that it is one that would allow inter-diffusion (e.g. between the inorganic shell) under aqueous conditions. In various embodiments, the organic polymer latex particles comprise water-dispersed organic polymer latex particles (no organic solvent). In various embodiments, the organic polymer latex particles comprise degradable polymer latex particles, biodegradable polymer latex particles, non toxic polymer latex particles, bioresorbable polymer latex particles, responsive polymer latex particles, stimuli-responsive polymer latex particles, thermo- responsive polymer latex particles, thermoplastic polymer latex particles, poly-N- isopropyl acrylamide (PNIPAM) latex particles, poly-methyl-methacrylate-co- poly-styrene-co-polyethyl-hexyl-acrylate-co-poly-acrylic acid latex particles, poly caprolactone (PCL) latex particles, poly valerolactone latex particles, poly butyrolactone latex particles, polyurethane latex particles, polyamide latex particles, polyacrylic acid-containing latex particles or combinations thereof. Advantageously, embodiments of the method produce capsules that are responsive to one or more stimuli that may be useful in stimuli-driven delivery applications. The organic polymer latex particles may optionally comprise a cross-linker optionally selected from bis-acrylates or acrylamides containing alkyl group or poly-ethylene group, or N,N’-Methylenebis(acrylamide) (BIS). In various embodiments, the heterocoagulating step is substantially devoid of the use/need of a cross-linker to form the organic polymer layer over the primary capsule. In some embodiments, where the organic polymer latex particles comprise poly caprolactone (PCL), the heterocoagulating step is carried out at a temperature of from about 60°Cto about 70°C,preferably 65°C,and/or without a cross-linker. In various embodiments, the organic polymer latex particles comprise no more than about 2% BIS, no more than about 1.5% BIS, no more than about 1.4% BIS, no more than about 1.3% BIS, no more than about 1.2% BIS, no more than about 1.1% BIS, no more than about 1.0% BIS, no more than about 0.9% BIS, no more than about 0.8% BIS, no more than about 0.7% BIS, no more than about 0.6% BIS, no more than about 0.5% BIS, no more than about 0.4% BIS, no more than about 0.3% BIS, no more than about 0.2% BIS or no more than about 0.1 % BIS.