Thirty-two ambient cured alkali-activated engineered composites (AAECs) were developed by incorporating MgO, multi-walled carbon nanotubes (MWCNTs), reduced graphene oxide (rGO), and polyvinyl alcohol (PVA) fiber with a one-part dry mix technique using powder-based activators/reagents. The effects of material variables, namely binary or ternary combination source materials (fly ash C or F and ground granulated blast furnace slag ‘GGBFS’), two types of reagents with varying chemical ratios and dosages of additives (from 0 to 5% MgO and from 0 to 6% MWCNT/rGO), on the physical (slump flow, flow time, flow velocity, and density), hardness (compressive strength from 0 to 180 days and 28-day ultrasonic pulse velocity ‘UPV’), and micro-structural (SEM/EDS, XRD and FTIR) properties were evaluated. All these variables, individually or combined, influenced the properties and microstructural aspects of AAECs. Problems associated with the dispersion and agglomeration of nanomaterials, which could disrupt the microstructure and weaken its mechanical/physical properties, were avoided through the use of defined ultra-sonication with a high-shear mixing protocol. All AAECs achieved a 28-day compressive strength ranging from 26.0 MPa to 48.5 MPa and a slump flow > 800 mm, satisfying the criteria for flowable structural concrete. The addition of 5% MgO and up to 0.3% MWCNT/rGO increased the compressive strength/UPV of AAECs with MgO-MWCNT or rGO combination provided an improved strength at a higher dosage of 0.6%. A linear correlation between compressive strength and UPV was derived. As per SEM/EDS and XRD analyses, besides common C-A-S-H/N-C-A-S-H or C-A-S-H/C-S-H gels, the addition of MgO led to the formation of magnesium-aluminum hydrotalcite (Ht) and M-S-H (demonstrating self-healing potential), while the incorporation of rGO produced zeolites which densified the matrix and increased the compressive strength/UPV of the AAECs. Fourier transform infrared spectrometer (FTIR) analysis also suggested the formation of an aluminosilicate network in the AAECs, indicating a more stable structure. The increased UPV of MWCNT/rGO-incorporated AAECs indicated their better conductivity and ability of self-sensing. The developed AAECs, incorporating carbon-nano materials and MgO additive, have satisfactory properties with self-healing/-sensing potentials.
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