Polydimethylsiloxane (PDMS) sponges incorporated with hydrophobic mesoporous silica nanoparticles (PDMS/H-MSNs) were fabricated by a sugar templating method. Hydrophobicity of H-MSNs was achieved by heat treatment under an inert atmosphere. PDMS/H-MSNs had a progressively increased water contact angle with loading amounts of H-MSNs. The mechanical properties were improved upon incorporation of H-MSNs in PDMS sponges. Also, PDMS/H-MSNs sponges were resilient as indicated by a complete recovery to its original shape after 50 cycles of compression strain at 50%. PDMS/H-MSNs sponges were capable of selectively absorbing diesel oil and various organic solvents. The sponges had the ability to completely remove solvents either floating on a water surface or under water. PDMS/H-MSNs increasingly absorbed chloroform with increasing amounts of H-MSNs with its absorption capacity as high as 2000%. The reusability was tested with PDMS/20H-MSNs sponges by repeated adsorption-desorption of dichloromethane. The sponge can maintain its absorption capacities after 20 adsorption-desorption cycles.