In the present work, a temperature and pH-responsive hybrid catalytic system using copolymer-capped mesoporous silica particles with metal nanoparticles is proposed. The poly(2-(dimethylamino)ethyl methacrylate)(DMAEMA)-co-N-tert-butyl acrylamide) (TBA)) shell on mesoporous silica SBA-15 was obtained through free radical polymerization. Then, copper nanoparticles (CuNPs) decorated SBA-15/copolymer hybrid materials were synthesized using the NaBH₄ reduction method. SBA-15 was functionalized with trimethoxylsilylpropyl methacrylate (TMSPM) and named TSBA. It was found that the CuNPs were uniformly dispersed in the mesoporous channels of SBA-15, and the hybrid catalyst exhibited excellent catalytic performance for the selective oxidation of different substituted benzyl alcohols in water using H₂O₂ as an oxidant at room temperature. The dual (temperature and pH-) responsive behaviors of the CuNPs/p(DMAEMA-co-TBA)/TSBA catalyst were investigated using the dynamic light scattering technique. The conversion of catalytic products and selectivity were calculated using gas chromatographic techniques, whereas the molecular structure of the products was identified using ¹H and ¹³C nuclear magnetic resonance (NMR) spectroscopy. The catalyst showed excellent catalytic activity toward the oxidation of alcohol to aldehyde in an aqueous medium below the lower critical solution temperature (LCST) and pKa values (7–7.5) of the copolymer. The main advantages of the hybrid catalyst, as compared to the existing catalysts, are outstanding alcohol conversion (up to 99%) for a short reaction time (1 h), small amount of the catalyst (5 mg), and good recyclability equal to at least five times.