Pickering Emulsions Research Articles

A double-layer film based on the strategy of tannic acid-anthocyanin co-pigmentation and tannic-crosslinked-gelatin/−reduced Ag nanoparticles for beef preservation and monitoring

A double-layer film was developed with tannic acid (TA) co-pigmented purple potato anthocyanin extract (PAE)-agar as the inner layer, and K-carrageenan-oregano essential oil Pickering emulsion (OPE)/silver nanoparticles (TA-AgNPs) as the outer layer. Molecular docking and FT-IR results elucidated that intermolecular hydrogen bond was the main interaction between components in the agar-carrageenan matrix, with TA and PAE contributing to intensified anthocyanin color through π-π stacking. The incorporation of OPE/TA-AgNPs enhanced the film's hydrophobicity (WCA > 100°) and UV–vis barrier (close to 0% at 200-320 nm, effectively impeding UVA, UVB, and UVC) properties and exhibited outstanding antioxidant (DPPH scavenging rate > 88%) and antimicrobial activities. This film showed a significant color change in the pH range of 2–12 (from pink to yellow) and a considerable sensitivity to volatile amines within 2 min. The films effectively alleviated beef spoilage (extending the shelf life of beef for 1d) and reflected the freshness of beef during storage. Additionally, the digital color information of the film was obtained by a smartphone combined with RGB values analysis to quantify the freshness of beef rapidly. Therefore, this study expands the application of food packaging films with freshness preservation and monitoring in the field of animal-derived food.

Preparation and Properties of Walnut Protein Isolate-Whey Protein Isolate Nanoparticles Stabilizing High Internal Phase Pickering Emulsions.

To enhance the functional properties of walnut protein isolate (WalPI), hydrophilic whey protein isolate (WPI) was selected to formulate WalPI-WPI nanoparticles (nano-WalPI-WPI) via a pH cycling technique. These nano-WalPI-WPI particles were subsequently employed to stabilize high internal phase Pickering emulsions (HIPEs). By adjusting the mass ratio of WalPI to WPI from 9:1 to 1:1, the resultant nano-WalPI-WPI exhibited sizes ranging from 70.98 to 124.57 nm, with a polydispersity index of less than 0.326. When the mass ratio of WalPI to WPI was 7:3, there were significant enhancements in various functional properties: the solubility, denaturation peak temperature, emulsifying activity index, and emulsifying stability index increased by 6.09 times, 0.54 °C, 318.94 m2/g, and 552.95 min, respectively, and the surface hydrophobicity decreased by 59.23%, compared with that of WalPI nanoparticles (nano-WalPI), with the best overall performance. The nano-WalPI-WPI were held together by hydrophobic interactions, hydrogen bonding, and electrostatic forces, which preserved the intact primary structure and improved resistance to structural changes during the neutralization process. The HIPEs stabilized by nano-WalPI-WPI exhibited an average droplet size of less than 30 μm, with droplets uniformly dispersed and maintaining an intact spherical structure, demonstrating superior storage stability. All HIPEs exhibited pseudoplastic behavior with good thixotropic properties. This study provides a theoretical foundation for enhancing the functional properties of hydrophobic proteins and introduces a novel approach for constructing emulsion systems stabilized by composite proteins as emulsifiers.

Sustained-release mechanism of β-Cyclodextrin/cationic cellulose-stabilized Pickering emulsions loaded with citrus essential oil

Citrus oil (CO) is a commonly used natural flavor with high volatility, which is not conducive to sustained release under food environmental stress. This study constructed novel β-cyclodextrin/cationic cellulose nanocrystal (β-CD/C-CNC) complexes via noncovalent interaction, which were used to stabilize CO-loaded Pickering emulsions (PEβ-CD/C-CNC). The C-CNC greatly improved the physical stability, droplet dispersion and viscoelasticity of PEβ-CD/C-CNC by forming a tight network structure, as verified by rheological behavior. Moreover, C-CNC improved the wettability of β-CD/C-CNC complexes and enhanced the interaction between adjacent β-CD/C-CNC complexes. C-CNC also contributed to the interfacial viscoelasticity, hydrated mass, and layer thickness via the interfacial dilational modulus and QCM-D. β-CD/C-CNC complexes adsorbed on the oil–water interface gave rise to a dense filling layer as a physical barrier, enhancing the sustained-release performance of PEβ-CD/C-CNC by limiting diffusion of citrus essential oil into the headspace. This study provides new technical approaches for aroma retention in the food industry.

Ozone induced structural variation in OSA waxy rice starch: Effects on the thermal behavior of starch and its stabilized pickering emulsion

Waxy rice starch (St) was modified by pre-OSA esterification reaction followed by ozone treatment. The molecular structure of this modified product (OSA-OSt) was characterized, and the thermal behaviors and its stabilized Pickering emulsion were evaluated. 1HNMR and XPS results discovered that ozone initially oxidized the hydroxyl groups in the amorphous region of starch (preferentially C2/C3) along with a degree of crosslinking, enhancing the molecular orderliness. This led to an increase in water-holding capability (29.15%) and swelling power (52.8 g/g), and a decrease in solubility (0.35%). TGA, RVA, and DSC indicated that oxidation-induced crosslinking within a brief treatment period enhanced the starch's thermal stability. The structural change enabled the formation of a weak gel structure during the heating process, which displayed high thermal and freeze-thaw stability. The work proves ozone is an effective way of improving the thermal behavior of OSA-starch and its emulsion for subsequent applications in numerous food products.

Relationship between the interfacial properties of lactoferrin-(−)-epigallocatechin-3-gallate covalent complex and the macroscopic properties of emulsions

This study explored the relationship between the interfacial behavior of lactoferrin-(−)-epigallocatechin-3-gallate covalent complex (LF-EGCG) and the stability of high internal phase Pickering emulsions (HIPPEs). The formation of covalent bond between lactoferrin and polyphenol was verified by the increase in molecular weight. In LF-EGCG group, the surface hydrophobicity, interfacial pressure, and adsorption rate were decreased, while the molecular flexibility, interfacial film viscoelasticity, and interfacial protein content were increased. Meanwhile, LF-EGCG HIPPE possessed reduced droplet size, increased ζ-potential and stability. Rheology showed the viscoelasticity, structural recovery and gel strength of LF-EGCG HIPPE were improved, giving HIPPE inks better 3D printing integrity and clarity. Moreover, the free fatty acids (FFA) release of LF-EGCG HIPPE (62.6%) was higher than that of the oil group (50.1%). Therefore, covalent treatment effectively improved the interfacial properties of protein particles and the stability of HIPPEs. The macroscopic properties of HIPPEs were positively regulated by the interfacial properties of protein particles. The result suggested that the stability of emulsions can be improved by regulating the interfacial properties of particles.

Bacterial microcompartment-mimicking Pickering emulsion droplets for detoxification of chemical threats under sweet conditions

Chemical warfare agents represent a severe threat to mankind and their efficient decontamination is a global necessity. However, traditional disposal strategies have limitations, including high energy consumption, use of aggressive reagents and generation of toxic byproducts. Here, inspired by the compartmentalized architecture and detoxification mechanism of bacterial micro-compartments, we constructed oil-in-water Pickering emulsion droplets stabilized by hydrogen-bonded organic framework immobilized cascade enzymes for decontaminating mustard gas simulant (2-chloroethyl ethyl sulfide, CEES) under sweet conditions. Two exemplified droplet systems were developed with two-enzyme (glucose oxidase/chloroperoxidase) and three-enzyme (invertase/glucose oxidase/chloroperoxidase) cascades, both achieving over 6-fold enhancement in decontamination efficiency compared with free enzymes and >99% selectivity towards non-toxic sulfoxide. We found that the favored mass transfer of sugars and CEES from their respective phases to approach the cascade enzymes located at the droplet surface and the facilitated substrate channeling between proximally immobilized enzymes were key factors in augmenting the decontamination efficacy. More importantly, the robustness of immobilized enzymes enabled easy reproduction of both the droplet formation and detoxification performance over 10 cycles, following long-term storage and in far-field locations.

Triply periodic minimal surfaces structured biphasic calcium phosphate bio-scaffolds with controllable porous struts from digital light processing of Pickering emulsion

Hierarchically porous biphasic calcium phosphate (BCP) ceramics with triply periodic minimal surface structure and porous framework have been fabricated by digital light processing (DLP) using dual-phase Pickering emulsion as the paste. The pristine hydroxyapatite and β-tricalcium phosphate particles were separately modified by dispersant firstly to obtain photosensitive Pickering emulsion with suitable rheological properties and stability for DLP printing. The porous structure has been well regulated by dispersant content, and ethylene glycol content. The resulting BCP ceramics exhibited a hierarchical pore structure consisting of interconnected micropores ranging from 1.13 μm to 8.98 μm and model-designed pores of nearly 500 μm, demonstrating excellent compressive strength of 4.83 MPa at a porosity of 60 %. In vitro biological experiments revealed that rat bone marrow mesenchymal stem cells exhibited good proliferation and adhesion ability on the BCP bio-scaffolds, thereby enhancing their application potential in bone regenerative medicine.

Colloidal lignin particle reinforces the stability of Pickering emulsions prepared with zein nanoparticle

Zein nanoparticle (ZNP) is at the forefront of research on Pickering emulsions, valued for its self-assembling and surfactant-free nature. Nevertheless, its emulsion stability is undermined by inadequate amphiphilicity. Colloidal lignin particle (CLP), characterized by its antithetical charge and amphiphilic nature, appears the promising for augmenting the stability of ZNP-based emulsion. This study meticulously investigated the impact of CLP on the colloidal properties and emulsifying performance of ZNP. The results revealed that electrostatic interactions between ZNP and CLP significantly mitigated the charge of ZNP and improved its hydrophilic/lipophilic balance. Under optimized conditions (1.0 wt% particle concentration, pH 4.0, 50% oil content), CLP notably reduced droplet sizes (41–225 μm) and enhanced the stability of ZNP-based Pickering emulsion, particularly at ZNP/CLP ratios of 6:4 and 5:5. In nature, CLP improved the stability ZNP-based Pickering emulsions via increased interfacial adsorption, enhanced steric hindrance, and reinforced viscous structure.

Effect of wet media milling on starch-quercetin complex: Enhancement of Pickering emulsifying ability and oxidative resistance

This research explored the effect of media milling on complexation of corn starch (CS) and quercetin (QC), interaction mechanism and Pickering emulsifying ability of corn-quercetin (CS-QC) complex. CS-QC with QC/CS ratio of 1:24 had the highest encapsulation efficiency of 76.00 ± 1.30 %. Average volume-mean diameter, average whole molecular size (Rh) and debranchedamylopectinchain length of CS-QC were significantly decreased after milling. Attenuated Total Reflectance-Fourier Transform Infrared spectroscopy (ATR-FTIR) and X-ray photoelectron spectroscopy (XPS) spectra confirmed the complexation between CS and QC. Emulsifying capacity and emulsion stability of Pickering emulsion stabilized by 5 % CS-QC complex particles after 120 min milling reached 100.00 % and 100.00. Pickering emulsions stabilized by these complex particles demonstrated superior oxidative stability. These results demonstrated that media milling could be an efficient physical approach to obtain starch-polyphenol complex by enhancing non-covalent interactions, which could not only be used as food-grade Pickering emulsifiers, but also retard lipid oxidation.

Quinoa starch-based Pickering emulsions with small-molecule oil solvents: Exploring solvent varieties and depletion attraction

The successful preparation of starch-based Pickering emulsions typically relies on the use of high-viscosity or high-boiling-point oil solvents. However, these solvents present challenges in removal and limit the applicability of the emulsions. This study aims to investigate the feasibility and effectiveness of employing small-molecule solvents as alternatives for the oil phase. Specifically, quinoa starch granules are used as the emulsifying agent, with a systematic exploration of various small molecules from different solvent categories. This research contributes by identifying the impact of solvent-particle interactions on the feasibility of emulsion formation—an aspect critical but often overlooked in previous discussions on solvent influence on emulsion quality, essential for guiding solvent selection. Furthermore, to address potential challenges associated with maintaining emulsion stability when using low-viscosity oils, a strategy based on exploiting depletion attraction is proposed and demonstrated, leveraging bovine serum albumin as depletants.

Development of Zanthoxylum bungeanum essential oil Pickering emulsions using potato protein-chitosan nanoparticles and its application in mandarin preservation

This study aimed to develop Pickering emulsions for the encapsulation of Zanthoxylum bungeanum essential oil (ZBEO) using potato protein-chitosan composite nanoparticles (PCCNs). The sustained release properties of ZBEO, antifungal efficacy, and preservation effects of formulated ZBEO-Pickering emulsions (ZBEO-PEs) on mandarins were evaluated. Particle size, zeta potential, emulsifying activity (EAI), and emulsifying stability (ESI) analysis showed that PCCNs prepared with the potato protein to chitosan mass ratio of 10:3 provided optimal emulsification and stabilization. Techniques such as differential scanning calorimetry (DSC), X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FT-IR) demonstrated that chitosan introduction increased the wettability of potato protein through electrostatic, hydrogen bonding, and hydrophobic interactions. ZBEO-PEs formulated with 3.0 % PCCNs and an oil fraction of 0.40 showed best encapsulation efficiency, storage stability and sustained release. Confocal laser scanning microscopy confirmed the adsorption of PCCNs, forming dense interface layers on the surface of oil droplets, thereby enhancing the stability of ZBEO-PEs. In vitro experiments demonstrated enhanced antifungal activity of ZBEO-PEs against Penicillium italicum and Penicillium digitatum. Additionally, storage experiments indicated that ZBEO-PEs coatings effectively controlled postharvest decay caused by Penicillium spp. in mandarins. Overall, the findings suggest that PCCNs are highly efficient emulsifiers for ZBEO Pickering emulsions, underscoring their potential as preservative coatings for mandarins.

Pickering emulsion via interfacial assembly of lignin particles and cationic surfactant: Formation of robust anchoring layer

Lignin, a byproduct of the paper and pulp industry, shows promise as stabilizers for emulsions, offering potential value-added applications to direct disposal. However, utilizing particulate lignin directly as stabilizers is challenging due to limited emulsion stability. In this study, co-stabilization of Pickering emulsions is investigated by combination of lignin particles and cationic surfactants (CTAB and DDAB), wherein lignin source and oil types are optimized with a focus on emulsion stability. A battery of characterization methods, including visual appearance, microstructure, droplet size, zeta potential, etc., is employed to evaluate emulsion stability. The findings reveal that kraft lignin nanospheres (LNS) are the optimal stabilizing particles. The incorporation of cationic surfactants via electrostatic adsorption enhances the stabilizing effect of LNS, and the use of DDAB is found to significantly enhance emulsion stability compared to CTAB, attributing to higher charge shielding capability of DDAB, as well as the formation of a more robust and compact nonpolar anchoring layer. The surfactant-assisted LNS can be used to stabilize a range of oil types, with tridecane as the optimal oil. This research presents a straightforward, efficient, and scalable approach for producing highly stable lignin-based Pickering emulsions, showing potential applications in recycling and value enhancement of waste lignin.

Preparation of polyurethane shell microcapsules containing isocyanate core by Pickering emulsion method using modified silica nanoparticles and investigation of their self-healing performance

Encapsulating repair agents are increasingly popular for repairing coating damage, with capsules being a common method to address surface scratches by releasing healing liquid into the fissure. However, creating microcapsules that are durable against environmental factors remains a key concern. Current research focuses on advancements in encapsulating healing agents and their production methods, particularly emphasizing the integration of capsules into coatings for external self-healing purposes. Polyurethane capsules containing isophorone diisocyanate were synthesized using the Pickering emulsion method with modified silica as a Pickering emulsion stabilizer in three different percentages and then dispersed in urea formaldehyde at varying weight percentages. The self-healing properties of this coating were then studied. Fourier transform infrared spectroscopy (FTIR), Soxhlet extraction, and thermogravimetric analysis (TGA) were performed on the samples to ensure the success of the encapsulation process. The morphology of the capsules was investigated using field emission scanning electron microscopy (FE-SEM), revealing that the synthesized capsules possess a spherical shape and are adequately spaced apart. These capsules were spherical at micron scales, with differences observed based on the quantity of stabilizing nanoparticles employed. Furthermore, the capsules demonstrated robust thermal stability, as evidenced by the increase in IPDI evaporation temperature from approximately 140 °C to 240 °C.Immersion test results in saltwater solutions showed that coatings containing pickering capsules exhibited better corrosion resistance, further validating the success of the research. The shell strength of the capsules prepared using the Pickering method was increased, enhancing the stability of the microcapsules during the mixing process with the resin and demonstrating self-healing properties. These findings have significant practical implications, as they demonstrate the potential to improve the durability and lifespan of coatings in various applications.

Double-layer films based on konjac gum and hydroxypropyl methyl cellulose loaded with thyme essential oil Pickering emulsion: Preparation, characterization, and application

Due to the challenges posed by petroleum-based plastics in terms of degradation and their contribution to environmental pollution, researchers have focused on natural biodegradable packaging materials. Herein, a biodegradable, unidirectional released, bilayer active film based on Konjac gum/hydroxypropyl methylcellulose (KGM/HPMC) were developed. Specifically, Pickering nano-emulsion was formed via ultrasonic self-assembly of Thyme essential oil (TEO) and a suspension of oxidized chitin nanocrystals. The dual-network form by KGM/HPMC effectively incorporated the TEO droplets in Pickering nano-emulsion through intermolecular hydrogen bonding, demonstrating good solubility between the TEO droplets and film matrix. The mechanical properties of the active film are greatly improved due to the protective effect provided by the outer layer in the double-layer active emulsion film design. Furthermore, the double-layer active film enables a unidirectional release of essential oils, thereby enhancing the efficiency of essential oil utilization. In addition, the double-layer active film has beneficial properties, including antioxidation, antibacterial effects, ultraviolet radiation protection, and biodegradability compared to cling film. This film was employed for the preservation of salmon, and the findings indicated that the bilayer active film, formulated with 15% Pickering emulsion content, notably retarded the escalation of total volatile basic nitrogen (TVB-N) and pH levels in salmon. Furthermore, it successfully reduced the proportion of dominant bacteria (specifically Pseudomonas) in salmon samples. The double-layer active film developed in this study demonstrates the potential for extending the shelf life of aquatic products.

Fabrication of thermo-responsive microcapsule pesticide delivery system from maleic anhydride-functionalized cellulose nanocrystals-stabilized pickering emulsion template

The overuse of pesticides has shown their malpractices. Novel and sustainable formulations have consequently attracted abundant attention but still appear to have drawbacks. Here, we use a maleic anhydride-functionalized cellulose nanocrystals-stabilized Pickering emulsions template to prepare thermo-responsive microcapsules for a pesticide delivery system via radical polymerization with N-isopropyl acrylamide. The microcapsules (MACNCs-g-NIPAM) are characterized by the microscope, SEM, FTIR, XRD, TG-DTG, and DSC techniques. Imidacloprid (IMI) is loaded on MACNCs-g-NIPAM to form smart release systems (IMI@MACNCs-g-NIPAM) with high encapsulation efficiency (~88.49%) and loading capability (~55.02%). The IMI@MACNCs-g-NIPAM present a significant thermo-responsiveness by comparing the release ratios at 35°C and 25°C (76.22% vs 50.78%). It also exhibits advantages in spreadability, retention and flush resistance on the leaf surface compared with the commercial IMI water-dispersible granules (CG). IMI@MACNCs-g-NIPAM also manifest a significant advantage over CG (11.12 mg/L vs 38.90 mg/L for LC50) regarding activity tests of targeted organisms. In addition, IMI@MACNCs-g-NIPAM has shown excellent biocompatibility and low toxicity. All the benefits mentioned above prove the excellent potential of IMI@MACNCs-g-NIPAM as a smart pesticide formulation.

Deep-Eutectic-Solvent-in-Water Pickering Emulsions Stabilized by Starch Nanoparticles.

Deep eutectic solvents (DESs) have received extensive attention in green chemistry because of their ease of preparation, cost-effectiveness, and low toxicity. Pickering emulsions offer advantages such as long-term stability, low toxicity, and environmental friendliness. The oil phase in some Pickering emulsions is composed of solvents, and DESs can serve as a more effective alternative to these solvents. The combination of DESs and Pickering emulsions can improve the applications of green chemistry by reducing the use of harmful chemicals and enhancing sustainability. In this study, a Pickering emulsion consisting of a DES (menthol:octanoic acid = 1:1) in water was prepared and stabilized using starch nanoparticles (SNPs). The emulsion was thoroughly characterized using various techniques, including optical microscopy, transmission microscopy, laser particle size analysis, and rheological measurements. The results demonstrated that the DES-in-water Pickering emulsion stabilized by the SNPs had excellent stability and retained its structural integrity for more than 200 days at room temperature (20 °C). This prolonged stability has significant implications for many applications, particularly in the field of storage and transportation. This Pickering emulsion based on DESs and SNPs is sustainable and stable, and it has great potential to improve green chemistry practices in various fields.

Lipase grafted on magnetic and CO2 dual-responsive Janus nanoparticles for interfacial catalyzed transesterification

Enzyme-loaded Pickering emulsions are a promising system for biphasic catalytic reactions. The monodisperse core-shell Janus nanoparticles (JNPs) P[xMAOAAO-yDEAEA]@RF@Fe3O4-CRL with magnetic and CO2 dual-responsiveness were synthesized by the wax/water emulsion. The catalysts can perfectly steady the oil/methanol Pickering emulsion and produce biodiesel by static transesterification of soybean oil. There is a synergistic effect between the interfacial activation of CRL realized by amphiphilic Janus supporters and the stability of the Pickering emulsions. Under optimal reaction conditions, the Pickering interfacial biocatalyst exhibits excellent enzymatic activity, reaching a biodiesel yield of 87.33 %. Furthermore, magnetic absorption and introduction of CO2 separate the catalyst P[2MAOAAO-DEAEA]@RF@Fe3O4-CRL from the system, and the biodiesel yield is 86.3 % after 6 cycles.

Pickering emulsions of zein nanoparticles co-stabilized by Tween 20: An effective strategy to stabilize citral in low pH environment

The demand for surfactant-free emulsions is growing significantly in food industry. Herein, we report the fabrication of zein nanoparticles, modified their surface hydrophobicity with Tween 20, and used them to stabilize various formulations of Pickering emulsions designated as ZT0 %, ZT5 %, ZT10 %, ZT15 %, ZT20 %, and ZT25 %, for preventing the acid-catalysed degradation of citral at 25 °C. Our results suggest that, as the concentration of Tween 20 increases, the droplet size of the emulsions first increases and then decreases, whereas the mechanical strength continuously increases. Citral encapsulated in ZT25 % shows maximum physicochemical stabilization as determined by visual, olfactory and HPLC analysis, and when released in saline shows maximum antioxidant activity due to the favorable charge characteristics on Pickering emulsifiers, and the existence of hydrophobic ⇋ electrostatic interaction. As compared to prior literature, our work represents a significant advancement in fabrication of zein nanoparticles (ZNPs), their stabilization using Tween 20 and the formation of appropriate Pickering emulsions stabilized by Tween 20 modified ZNPs appropriate for modifying the interfacial characteristics of the emulsion for enhanced physicochemical stability, excellent aroma profile, controlled release rate, and improved antioxidant activity of encapsulated citral under harsh acidic conditions. Moreover, the novel Chemical Kinetic Method has been applied to analyze and interpret the citral stability as a function of interfacial parameters. The study, therefore presents a novel particle-surfactant complex interface, having great potential for the encapsulation, protection, and release of citral from the acidic food/pharmaceutical formulations.

Quercetin encapsulation and release using rapid CO2-responsive rosin-based surfactants in Pickering emulsions

Emulsion-based delivery systems are extensively employed for encapsulating functional active ingredients, protecting them from degradation, and enhancing bioavailability and release efficiency. Here, a CO2-responsive surfactant synthesized from rosin displays rapid responsiveness to CO2 at room temperature, transitioning reversibly switches between active and inactive states multiple times. The dual tertiary amines on the rosin rigid structure contributes to its CO2 sensitivity. When in its active cationic form, in conjunction with silica nanoparticles, it exhibits desired Pickering emulsification performance across various oil phases. In the Pickering emulsion loaded with quercetin, the encapsulation efficiency and loading efficiency reached 80.50% and 0.69%, respectively, with stability lasting at least 30 days. The system provides robust protection for quercetin against external factors, such as UV and heat, revealing sustained release effects. This study investigated the potential of using rosin-based CO2-responsive surfactants alongside nanoparticles to design stable Pickering emulsion systems for active substance encapsulation and sustained release.

Statistical Copolymerization-Induced Self-Assembly.

Statistical copolymers have been extensively used in chemical industries and our daily lives, owing to their ease of synthesis and functionalization. However, self-assembly based on statistical copolymers has been haunted by high interfacial energy, poor stability, and low concentration. We proposed the statistical copolymerization-induced self-assembly (stat-PISA) as a general strategy for one-step preparing stable statistical copolymer assemblies with high solids content. The concept was demonstrated through a model dispersion polymerization system comprising a charged hydrophilic monomer and a core-forming monomer, producing spherical micelles via a spinodal decomposition mechanism with an interconnected network intermediate. The stat-PISA was tunable by varying the fraction of charged monomer, the polymer chain length, and the solids content. The statistical copolymer micelles were demonstrated to be a potential Pickering emulsifier with superior stabilizing performances compared to their block copolymer counterparts. The general applicability of stat-PISA was demonstrated by preparing statistical copolymer assemblies with varying surface charges and chemical compositions. Particularly, this strategy is feasible for conventional free radical polymerization, promising for industrial scale-up.