Redox Responsiveness Research Articles

Redox responsive paclitaxel dimer for programmed drug release and selectively killing cancer cells

Redox stimulus responsive drug delivery systems have been widely investigated and proved to be promising prospects for efficient cancer therapy due to the abnormal high level of reactive oxygen species and glutathione in tumor microenvironment. Herein, three paclitaxel dimers (named as PTX2-R, R = S, Se and Te) bridged with alkyl sulfide, selenide or telluride are synthesized. These dimers can self-assemble into stable uniform nanoparticles (named as PTX2-R NPs, R = S, Se and Te) with impressively high drug loading. As expected, sulfur/selenium/tellurium bonds exhibit different redox responsiveness, thereby affecting the drug release and cytotoxicity. Of note, tellurium bridged paclitaxel dimer shows ultra-sensitivity to hydrogen peroxide, which rapidly cleaves into two paclitaxel under the subsequent dithiothreitol stimulation. Our findings provide deep insight into the redox sensitivity of chalcogenide elements and offer the rational design strategies to biologically redox condition for programmed drug release.

Preparation of redox responsive modified xanthan gum nanoparticles and the drug controlled release

A new kind of redox responsive nanoparticles was prepared through the modification and crosslinking reaction of xanthan gum. The nanoparticles had regular spherical shapes with diameters ranging from 110 to 180 nm. The nanoparticles showed good redox responsiveness. Doxorubicin (DOX) was loaded in the nanoparticles via ionic interaction with SO3 -, for increasing the drug loading rate and avoiding drug leakage. The in vitro drug release could be controlled by pH and reduction conditions simulated to the internal environment of tumor cells. The nanoparticles were biocompatible and could be potentially applied as anti-cancer drug vehicles for targeted release.

Enhanced cytotoxicity of a redox-sensitive hyaluronic acid-based nanomedicine toward different oncocytes via various internalization mechanisms

Receptor-mediated active targeting and tumor microenvironment responsive systems from polymeric micelles have been studied for rapid cellular internalization and triggered drug release. Previously we have constructed redox-responsive polymeric micelles composed of vitamin E succinate conjugated hyaluronic acid (HA-ss-TOS), which are able to actively target CD44 proteins and quickly release loaded drugs upon exposure to high levels of glutathione (GSH) in tumor cells. In the present study, we found that despite different cellular internalization mechanisms, micelles showed strong antineoplastic effects on 4T1 and B16F10 cells due to redox responsiveness. HA-ss-TOS-PTX micelles exhibited an excellent tumor targeting ability and prolonged retention time compared to Taxol in vivo. In addition, a superior antitumor effect was achieved compared to PTX-loaded insensitive micelles (HA-TOS-PTX) and Taxol. Our results revealed that PTX-loaded HA-ss-TOS micelles could enhance the antineoplastic efficacy of PTX for breast cancer and melanoma treatment and, thus, deserve further attention.

Actively Targeted and Redox Responsive Delivery of Anticancer Drug by Chitosan Nanoparticles.

The clinical efficacy of methotrexate (MTX) is limited by its poor water solubility, its low bioavailability, and the development of resistance in cancer cells. Herein, we developed novel folate redox-responsive chitosan (FTC) nanoparticles for intracellular MTX delivery. l-Cysteine and folic acid molecules were selected to be covalently linked to chitosan in order to confer it redox responsiveness and active targeting of folate receptors (FRs). NPs based on these novel polymers could possess tumor specificity and a controlled drug release due to the overexpression of FRs and high concentration of reductive agents in the microenvironment of cancer cells. Nanoparticles (NPs) were prepared using an ionotropic gelation technique and characterized in terms of size, morphology, and loading capacity. In vitro drug release profiles exhibited a glutathione (GSH) dependence. In the normal physiological environment, NPs maintained good stability, whereas, in a reducing environment similar to tumor cells, the encapsulated MTX was promptly released. The anticancer activity of MTX-loaded FTC-NPs was also studied by incubating HeLa cells with formulations for various time and concentration intervals. A significant reduction in viability was observed in a dose- and time-dependent manner. In particular, FTC-NPs showed a better inhibition effect on HeLa cancer cell proliferation compared to non-target chitosan-based NPs used as control. The selective cellular uptake of FTC-NPs via FRs was evaluated and confirmed by fluorescence microscopy. Overall, the designed NPs provide an attractive strategy and potential platform for efficient intracellular anticancer drug delivery.

Catalase, glutathione, and protein phosphatase 2A-dependent organellar redox signalling regulate aphid fecundity under moderate and high irradiance.

Redox processes regulate plant/insect responses, but the precise roles of environmental triggers and specific molecular components remain poorly defined. Aphid fecundity and plant responses were therefore measured in Arabidopsis thaliana mutants deficient in either catalase 2 (cat2), different protein phosphatase 2A (PP2A) subunits or glutathione (cad2, pad2, and clt1) under either moderate (250 μmol m-2 s-1 ) or high (800 μmol m-2 s-1 ) light. Aphid fecundity was decreased in pp2a-b'γ, cat2 and the cat2 pp2a-b'γ double mutants relative to the wild type under moderate irradiance. High light decreased aphid numbers in all genotypes except for cat2. Aphid fecundity was similar in the cat2 and glutathione-, phytoalexin-, and glucosinolate-deficient cat2cad2 double mutants under both irradiances. Aphid-induced increases in transcripts encoding the abscisic acid-related ARABIDOPSIS ZINC-FINGER PROTEIN 1 transcription factor were observed only under moderate light. Conversely, aphid induced increases in transcripts encoding the jasmonate-synthesis enzyme ALLENE OXIDE CYCLASE 3 was observed in all genotypes only under high light. Aphid-induced increases in REDOX RESPONSIVE TRANSCRIPTION FACTOR 1 mRNAs were observed in all genotypes except pp2a-b'ζ1-1 under both irradiances. Aphid fecundity is therefore regulated by cellular redox signalling that is mediated, at least in part, through PP2A-dependent mitochondria to nucleus signalling pathways.

Selenide-containing soluble polyimides: High refractive index and redox responsiveness

Soluble high refractive index polyimides have extensive applications in optical devices due to their ease of processing and versatility. In this work, selenide-containing polyimides were designed and synthesized via amine-dianhydride polycondensation. Two selenide containing diamines, e.g. bis(3-trifluoromethyl-4-aminophenyl)selenide (BTFAPS) and bis(4-aminophenyl)selenide (BAPS) were reacted with 4,4′-(Hexafluoroisopropylidene)diphthalic anhydride (6FDA) for the preparation of selenide containing polyimides. Comparison with its oxygen and sulfur counterparts, the selenide-containing PIs have better solubility, higher refractive index, and can bring redox responsiveness. This is due to the trifluoromethyl base, which possesses a large free volume, and the selenium element, which has a higher molar refraction and redox activities than even sulfur. Various techniques, such as nuclear magnetic resonance, gel permeation chromatography, Fourier transformed infrared spectroscopy and wide angle X-ray diffraction were used for characterizing the polymers structure. Differential scanning calorimetry, thermogravimetric analysis, ultraviolet-visible spectroscopy, spectroscopic ellipsometry and X-ray photoelectron spectroscopy were used to characterize the properties of the polymers.

Reversible Redox Switching of Concurrent Luminescence and Visual Color Change Based on Lanthanide Metallogel.

The development of reversible redox supramolecular gels capable of concurrent luminescence switch and visible color change with the facile redox process has always been an intriguing challenge. A redox-responsive supramolecular lanthanide metallogel with strong luminescence and yellow color is obtained via coordination interaction between 3,5-dinitrosalicylic acid (DNSA) and europium (Eu3+). Upon the addition of TiO2 to the prepared gel (DNSA/Eu3+ gel), the oxidation process of the gel (DNSA/Eu3+/TiO2 gel) can be easily achieved by UV irradiation. The DNSA/Eu3+/TiO2 gel exhibits a concurrent reversible "on-off" luminescence and color change in response to redox stimuli. The DNSA/Eu3+/TiO2 gel shows a concurrent quench of luminescence and a color change from yellow to red when the gel was stimulated by the reductant. Upon UV irradiation, the luminescence and color of the reduced DNSA/Eu3+/TiO2 gel restored to its initial state due to the strong oxidation ability of hydroxyl radicals derived from photocatalytic oxidation of TiO2. The results of UV-vis and mass spectroscopy indicated that the reversible redox responsiveness of DNSA/Eu3+/TiO2 gel depends on the reversible oxidation-reduction reactions of DNSA. Moreover, DNSA/Eu3+/TiO2 gel remains stable because the morphology of the gel had no change during the redox process. Exemplarily, the application of DNSA/Eu3+/TiO2 gels to achieve luminescent patterning was investigated. The results demonstrated that the prepared metallogel has potential applications in the fields of writable materials, anticounterfeiting, sensors, and others.

Redox-Sensitive Polymer Micelles Based on CD44 and Folic Acid Receptor for Intracellular Drug Delivery and Drug Controlled Release in Cancer Therapy.

Redox-responsive ferrocene (Fc)-grafted supramolecular block copolymers functionalized with hyaluronic acid (HA-g-β-CD/Fc-polymers or HAP) or folic acid (FA-g-β-CD/Fc-polymers or FAP) were synthesized by host-guest interaction. The copolymer structures were characterized by Fourier transform infrared spectroscopy, nuclear magnetic resonance, and gel permeation chromatography. The block copolymers self-assemble into spherical micellar aggregates in aqueous solution, and exhibit reversible redox characteristics in the presence of an oxidant and reductant. The tunable redox response was evaluated by transmission electron microscopy, ultraviolet-visible spectroscopy, cyclic voltammetry and dynamic light scattering. The micelles rapidly release DOX under oxidative and acidic condition in vitro. Furthermore, presence of HA and FA on the micelles enabled effective uptake by the CD44 and FA receptor-overexpressing cancer cells. Taken together, the redox responsive Fc-block copolymer micelles have good biocompatibility, biodegradability, low toxicity, and high selectivity, and are a highly promising drug delivery system for cancer therapy.

Reductive response and RGD targeting nano-graphene oxide drug delivery system

Cancer cell therapy using redox response and targeted drug delivery systems can increase therapeutic effects of anti-cancer therapy. Here, we report a redox-responsive drug carrier based on nanoscale Graphene Oxide (GO) loaded with Doxorubicin (DOX). In this drug carrier demonstration, we utilized Arginine-glycine-aspartic acid (RGD) peptide, aminated polyethylene glycol (6ARM-PEG-NH2, PEG-NH2) to functionalize the GO. To integrate the carrier with a redox responsive property, we utilized disulfide linkages (3,3′-dithiodipropionic acid (DTPA)), which can be cleaved by glutathione (GSH) combined with the PEG-NH2. Our results show that DOX is rapidly released in a pH = 5.50 PBS solution with GSH concentration of 10 mM. The drug-loading system (RGD-GO-PEG-S-S-DOX) combined with photo-thermotherapy possesses good inhibition activity of Hep-G2 cells at a relatively low concentration. When the concentration of RGD-GO-PEG-S-S-DOX was 1.56 μg/mL, the inhibition activity of Hep-G2 cells was 78%. Because tumor cells generally exhibit a higher concentration of GSH than normal ones, and tumor blood vessels are distorted and dilated, and the blood flow resistance tends to be large, tumor cells are more sensitive to temperature changes than normal tissues. Thus, drug delivery systems, like the one we studied, have potential applications in a therapeutic strategy for the treatment of liver cancer.

PH/Redox-Controlled Interaction between Lipid Membranes and Peptide Derivatives with a "Helmet".

How to reduce the cytotoxicity of antitumor peptides to normal cells remains an ongoing challenge. Here, we designed a pH/redox-responsive supramolecular structure (Pep-V⊂P-PEG) composed of a peptide modified with viologen (Pep-V) and polyethylene glycol bearing pillar[5]arene (P-PEG) as a "helmet". By shielding the hydrophobic moiety of the peptide derivative with pillar[5]arene via host-guest interactions, its disruption on normal cells can be effectively reduced. At acidic pH, the supramolecular structure can selectively adsorb onto negatively charged lipid membranes because of electrostatic interactions. Owing to redox responsiveness of the viologen group, Pep-V could be separated from P-PEG after the addition of reductants and inserted into lipid bilayers, which leads to membrane disruption. Cargo leakage of liposome models was investigated to understand Pep-V⊂P-PEG-induced liposomal membrane disruption under different pH values and redox conditions. Results showed that Pep-V⊂P-PEG caused almost no cargo leakage from (1,2-dipalmitoyl-sn-glycerol-3-phosphocholine) liposomes at pH 7.4 but significant leakage from negatively charged (1,2-dipalmitoyl-sn-glycerol-3-phospho-(1-rac-glyerol)) liposomes at pH 5.0 under a reducing environment. Pep-V⊂P-PEG displayed low destructive effects on mimic normal cells and significant disruption to mimic tumor cells when exposed to a reducing environment that is expected to be a potential antitumor agent.

Anion Exchange Membranes with Dynamic Redox-Responsive Properties.

Redox-responsive anion exchange membranes were developed using photoinitiated free-radical polymerization and reversible oxidation and reduction of viologen. The membranes were formulated using poly(ethylene glycol diacrylate) and diurethane dimethacrylate oligomers, dipentaerythritol penta-/hexa-acrylate cross-linker, photoinitiators, and 4-vinylbenzyl chloride as precursors for functionalization. In the membrane, 4,4'-bipyridine reacted with the 4-vinylbenzyl chloride residues, and subsequently, unreacted amines were methylated with iodomethane to obtain viologen as both the ion carrier and redox-responsive group. Upon oxidation, viologen supports two cations, where the reduced form only contains one cation. Thus, the redox responsiveness changed the membrane ionicity by a factor of 2. The area-specific resistance of the membranes in the oxidized, +2, state was lower than in the reduced, +1, state. The resistance increased between 40.6 ± 0.1 and 111.6 ± 0.1%, depending on membrane thickness, with the most significant increment being a resistance change from 4.88 × 10-4 Ω m2 in the oxidized state to 1.03 × 10-3 Ω m2 in the reduced state. Membrane permselectivity in the reduced, +1, state was between 15.9 ± 0.1 and 26.5 ± 0.01% lower than in the oxidized, +2, state, with no change in water uptake, spanning an average of 0.87 ± 0.02 in the oxidized state to an average of 0.7 ± 0.01 in the reduced state. Upon reduction, membrane ion-exchange capacity decreases, increasing ionic resistance and decreasing membrane permselectivity due to a reduction in fixed charge concentration without a measurable change in water uptake. This trend is not generally observed for ion-exchange membranes and explains that the changes in transport properties result from changes in ionicity, not water uptake or domain size. The reversibility and stability of the stimuli responsiveness were confirmed by the absence of transport property changes after redox cycling.

DOX-Conjugated keratin nanoparticles for pH-Sensitive drug delivery

Keratin is a good candidate for drug carrier due to its good biocompatibility, low immunogenicity, redox responsiveness, and abundant renewable sources. Herein, doxorubicin (DOX) was first conjugated with keratin through a pH-sensitive hydrazone linkage, and then prepared into particulate drug carrier via desolvation method. The size, morphology, and surface potential of keratin-DOX nanoparticles (KDNPs) were characterized by dynamic light scattering (DLS) and transmission electron microscopy (TEM). The drug release results showed that KDNPs performed an excellent pH-sensitive behavior under acidic tumor microenvironment. Cytotoxicity assay by MTT confirmed that KDNPs exhibited the enhanced cytotoxicity against A549 cells. Furthermore, KDNPs had higher therapeutic efficiency in vivo than free DOX. Hemolysis assay indicated that KDNPs was blood compatible. All the results identified that KDNPs are well suited as an ideal drug carrier.

Vinblastine-Loaded Nanoparticles with Enhanced Tumor-Targeting Efficiency and Decreasing Toxicity: Developed by One-Step Molecular Imprinting Process.

Molecularly imprinted polymers have exhibited good performance as carriers on drug loading and sustained release. In this paper, vinblastine (VBL)-loaded polymeric nanoparticles (VBL-NPs) were prepared by a one-step molecular imprinting process, avoiding the waste and incomplete removal of the template, and evaluated as targeting carriers for VBL delivery after modification. Using acryloyl amino acid comonomers and disulfide cross-linkers, VBL-NPs were synthesized and then conjugated with poly(ethylene glycol)-folate. The dynamic size of the obtained VBL-NPs-PEG-FA was 258.3 nm (PDI = 0.250), and the encapsulation efficiency was 45.82 ± 1.45%. The nanoparticles of VBL-NPs-PEG-FA were able to completely release VBL during 48 h under a mimic tumor intracellular condition (pH 4.5, 10 mM glutathione (GSH)), displaying significant redox responsiveness, whereas the release rates were much slower in the mimic body liquid (pH 7.4, 2 μM GSH) and tumor extracellular environment (pH 6.5, 2 μM GSH). Furthermore, the carriers NPs-PEG-FA, prepared without VBL, showed satisfactory intrinsic hemocompatibility, cellular compatibility, and tumor-targeting properties: they could rapidly and efficiently accumulate to folate receptor positive Hela cells and then internalized via receptor-mediated endocytosis, and the retention in tumor tissues could last for over 48 h. Interestingly, VBL-NPs-PEG-FA could evidently increase the accumulation of VBL in tumor tissues while decreasing the distribution of VBL in organs, exert similar anticancer efficacy against Hela tumors in the xenograft model of nude mice to VBL injection, and significantly improve the abnormality of liver and spleen observed in VBL injection. VBL-NPs-PEG-FA has the potential to be the delivery carrier for VBL by enhancing the tumor-targeting efficacy of VBL and decreasing toxicity to normal tissues.

Multifunctional drug carrier based on PEI derivatives loaded with small interfering RNA for therapy of liver cancer

Gene therapy strategies for liver cancer have broad application prospects but still lack a stable and efficient delivery vehicle. To overcome this obstacle, we designed a multifunctional gene delivery vector, sTPssOLP, which was based on oleylamine (OA)-modified disulfide-containing polyethylenimine (PEI) and incorporated into lipids to prepare a lipid nanoparticle. sTPssOLP consisted of the core of PEI derivative and cationic lipids bound to siRNA. The modified polyethylene glycol (PEG) and transferrin (Tf) were partially embedded in the phospholipid bilayer through the lipid and the other as the outer shell. The aim was to use the redox responsiveness of disulfide to trigger siRNA release in cytoplasm to enhance transfection efficiency. Pegylated lipids and Tf focus on increasing cycle life in the body and increasing accumulation at the tumor site of the carrier. In addition, two vectors were prepared as controls, one based on a PEI derivative containing no disulfide bond (POLP) and the other on the surface of the carrier not linked to Tf (PssOLP). PEI derivatives effectively avoid the toxicity problems caused by the use of PEI alone (25 kDa). Meanwhile, it was confirmed by gel retardation experiments that in the presence of dithiothreitol (DTT), the disulfide bond can indeed be reduced and the siRNA entrapped in the vector can be released. Both HepG2 and SMMC had significant uptake of sTPssOLP. The results of intracellular and lysosomal co-localization indicated that sTPssOLP achieved lysosomal escape. RT-PCR and Western blot results also confirmed that sTPssOLP had the best gene silencing activity. In vivo, the tumor inhibition rate of sTPssOLP in nude mice carrying HepG2 xenografts was 56%, which was significantly greater than that of the saline control group. In vivo imaging results showed that fluorescently labeled siRNA loaded in sTPssOLP was able to deliver more to the tumor site. At the same time, it was observed that sTPssOLP did not show significant damage to normal tissues. Therefore, this multifunctional gene delivery vector warrants further investigation.

Ultrasmall MoS2 Nanodots-Doped Biodegradable SiO2 Nanoparticles for Clearable FL/CT/MSOT Imaging-Guided PTT/PDT Combination Tumor Therapy.

Recently, we developed ultrasmall molybdenum disulfide (MoS2) quantum dots for computed tomography (CT) and multispectral optoacoustic tomography (MSOT) imaging-guided photothermal therapy (PTT). But, due to rapid body elimination and limited blood circulation time, the tumor uptake of the dots is low. In our study, this problem was solved via designing an amino-modified biodegradable nanomaterial based on MoS2 quantum-dots-doped disulfide-based SiO2 nanoparticles (denoted MoS2@ss-SiO2) for multimodal application. By integrating the MoS2 quantum dots into clearable SiO2 nanoparticles, this nanoplatform with an appropriate particle size can not only degrade and excrete in a reasonable period induced by redox responsiveness of glutathione but also exhibit a high tumor uptake due to the longer blood circulation time. Moreover, hyaluronic acid and chlorin e6 (Ce6) were adsorbed on the outer shell for tumor-targeting effect and photodynamic therapy, respectively. So, this biodegradable and clearable theranostic nanocomposite, which is applicable in integrated fluorescence/CT/MSOT imaging-guided combined photothermal therapy (PTT) and photodynamic therapy, is very promising in biomedical applications in the future.

Synthesis of multifunctional miktoarm star polymers via an RGD peptide-based RAFT agent

A “grafting from” approach for facile access of multifunctional miktoarm star polymers containing peptide arms.

Dimeric Prodrug Self-Delivery Nanoparticles with Enhanced Drug Loading and Bioreduction Responsiveness for Targeted Cancer Therapy.

Efficient drug accumulation in tumor cells is essential for cancer therapy. Herein, we developed dimeric prodrug self-delivery nanoparticles (NPs) with enhanced drug loading and bioreduction responsiveness for triple negative breast cancer (TNBC) therapy. Specially designed camptothecin dimeric prodrug (CPTD) containing a disulfide bond was constructed to realize intracellular redox potential controlled drug release. Direct conjugation of hydrophobic CPTD to poly(ethylene glycol) PEG5000, a prodrug-based amphiphilic CPTD-PEG5000 co-polymer was synthesized, which could encapsulate parental CPTD prodrug spontaneously and form ultrastable NPs due to the highly analogous structure. Such dimeric prodrug self-delivery nanoparticles showed ultrahigh stability with critical micelle concentration as low as 0.75 μg/mL and remained intact during endocytosis. In addition, neurotensin (NT), a 13 amino acid ligand, was further modified on the nanoparticles for triple negative breast cancer (TNBC) targeting. Optimized NT-CPTD NPs showed improved pharmacokinetics profile and increased drug accumulation in TNBC lesions than free CPT, which largely reduced the systemic toxicity and presented an improved anticancer efficacy in vivo. In summary, with advantages of extremely high drug loading capacity, tumor microenvironmental redox responsiveness, and targeted TNBC accumulation, NT-CPTD NPs showed their potential for effective triple negative breast cancer therapy.

Self-assembly of two ferrocence- and α-cyclodextrin-derived unconventional amphiphiles with redox responsiveness

We report the self-assembly of two α-cyclodextrin-derived unconventional amphiphiles containing a ferrocence and a ferrocenium terminal group (Fc-EG-αCD and Fc+-EG-αCD), respectively. Fc-EG-αCD was synthesized and then oxidized giving the oxidized state molecule Fc+-EG-αCD. The self-assembly behaviors of the molecules were investigated by several complementary techniques including TEM observations, DLS and other spectral measurements. Vesicles were formed in both systems. However, they adopted different molecular arrangements due to the varied electric properties of Fc and Fc+. Moreover, the reversibility of the redox-responsive self-assembly was successfully achieved. Our results enriches the self-assembly systems based on CD derivatives and provides a new route for the fabrication of more stimuli-responsive amphiphilic self-assemblies.

Reversing Redox Responsiveness of Hydrogels due to Supramolecular Interactions by Utilizing Double-Network Structures.

Stimuli-responsive hydrogels have been actively researched, and some of them have been put into practical use. When we create and use stimuli-responsive hydrogel materials, controlling stimuli responsiveness of hydrogels is a very important issue. In this research, we prepared hydrogels having single-network (SN) or double-network (DN) gel structures with the host-guest interaction groups cyclodextrin and methyl viologen and evaluated their stimuli responsiveness. The results of the tensile and compression tests showed that the hydrogels with SN and DN structures exhibited opposite stimuli responsiveness in response to the redox reaction of methyl viologen through the association and dissociation of the host molecule, β-cyclodextrin, and the guest molecule, methyl viologen. Spectroscopic measurements and rheological studies all indicated that this difference in stimuli responsiveness originated from the polymer-network structures. In addition, a chemically cross-linked DN gel was prepared and its redox responsiveness was evaluated.

Ferrocene-Containing Inverse Opals by Melt-Shear Organization of Core/Shell Particles.

In this work, the preparation of redox-responsive elastomeric inverse opal films featuring switchable structural colors is reported. The pristine core/shell particle architecture consists of a silica core having a metallopolymer shell, that is, poly(2-(methacryloyloxy)ethyl ferrocene carboxylate) (PFcMA) copolymerized with n-butyl methacrylate (PFcMA-co-PnBuMA) synthesized via seeded and stepwise emulsion polymerization protocols. This tailor-made, inorganic core/hybrid organic shell architecture leads to monodisperse particles, which were then subjected to the so-called melt-shear organization technique. After a cross-linking reaction and the core particle removal, vivid structural colors are obtained due to the well-ordered voids within the metallopolymer-containing matrix. In addition, redox responsiveness is shown by the addition of chemical oxidation and reducing agents as well as by cyclic voltammetry studies, thus revealing both a change of surface wettability and a change of the structural reflection colors. Herein, the described one-pot strategies for the preparation of metallopolymer-containing core/shell hybrid particles and application of the melt-shear ordering technique paves the way to novel redox-responsive porous opal films, which are expected to be promising materials in the field of remote-switchable sensors or electrochemical adsorbents.