We report new flexible “marshmallow-like” aerogels and xerogels with a bendable feature from the methyltrimethoxysilane (MTMS) and dimethyldimethoxysilane (DMDMS) co-precursor systems. A 2-step acid/base sol–gel process and surfactant are employed to control the phase separation of the hydrophobic networks, which give porous monolithic gels. The obtained gels become softer and more flexible with increasing DMDMS fractions.