Poly(methylmethacrylate)(PMMA)-modified silica aerogels were prepared via sol–gel synthesis followed by ambient pressure drying through hydrolysis and polycondensation of sodium silicate as a precursor. (3-trimethoxysilyl)propyl methacryloxy (TMSPM) was employed as the bonding between PMMA and nanoparticles of the aerogels skeletal backbone for avoid PMMA leaching. We studied the effects of various contents of polymer and TMSPM on the physico-chemical properties of the silica aerogels. The resulting polymer coatings increase the density of the aerogels by a factor of 2–3 but the Yong's modulus and hardness of the resulting materials may increase by more than 12 and 61 orders of magnitude. Modified by 30% PMMA and 15 ml TMSPM, the aerogel ultimately failed at 60% compressive strain and the final compressive stress is 168 MPa according to the compressing test. It was found that the nanoporous structure of aerogels could be well protected by introducing PMMA into the silica network.