Influence of noncovalent surface modification of multiwalled carbon nanotube (MWCNT) by ionic liquid on the surface characteristics and wetting behavior of nanocomposites were investigated using contact angle 56measurements with water and dimethyl sulfoxide. The surface energy, work of adhesion, polarity, spreading coefficient, interfacial energy, and interaction parameter were measured for all composites. This chapter is presented as (1) contact angle studies of styrene-butadiene rubber (SBR)/f-MWCNT nanocomposites—effect of MWCNT loading and (2) contact angle studies of SBR/f-MWCNT nanocomposites—effect of ionic liquid loading. The wetting property shows that contact angle of water droplets on a sample surface is increased from ~87° (SBR surface) to ~105° (SBR with 5 phr f-MWCNT). Enhancement in hydrophilicity of the SBR nanocomposite films has been observed at higher ionic liquid concentration is attributed to increase in surface energy due to the incorporation of polar groups on the films surface. Tunable surface characteristics are obtained by controlling the chemical structure and composition of the polymer surfaces.