Previous investigations on voltage-activated adhesives were restricted to aqueous solvents, where current directed crosslinking competed with water electrolysis.Replacing aqueous would expand applications of electrocuring technology and avoid excessive foaming, but many organic solvents have high ohmic resistances that prevent electrical conduction. These impediments were overcome through internal grafting of ferrocene (Fc) and diazirine (Dz) donor-acceptor pairs on fifth generation polyamidoamine (G5-PAMAM) dendrimers, forming G5-Fc-Dz cografted conjugates, where Fc internal additives provided an instantaneous conductive hole (+) network towards the redox conversion of diazirine to carbene insertion adhesion in non-toxic organic solvents of DMSO, DMF, and PEG400. Size exclusion chromatography and 1 H, 19 F NMR evaluated the formulations before and after electrocuring to quantitate grafting ratios and crosslinked dendrimers. Cyclic voltammetry confirmed the retained redox behavior of grafted Fc and Dz.Real-time electro-rheology established the dependence of crosslinking kinetics and adhesion strength on applied voltage. Liquid G5-Fc 15 -Dz 30 conjugates reached gelation within 2 min and with a storage modulus up to 3.4 ± 0.5 kPa. For the first time, a model system demonstrates the design components necessary towards organic, voltage-activated one-pot adhesives. This has broad implications for adhesives, cosmetics, implantable biomaterials, and flexible biosensors.