Light-driven liquid crystalline elastomer (LCE) composites with thiol-functionalized Ti3C2Tx MXene nanosheets are introduced as a versatile material system for achieving controlled locomotion. By incorporating superhydrophobic or superhydrophilic coatings, these composites demonstrate distinct modalities at the air-water interface and underwater. The stimuli-responsive behavior of the LCE nanocomposites is enhanced through the homogeneous dispersion of MXene platelets within the LCE matrix, facilitated by thiol-functionalization. Superhydrophobic coatings increase buoyancy and reduce drag, enabling locomotion akin to water striders at the air-water interface. Conversely, superhydrophilic coatings submerse the composites, allowing photomechanical actuation to drive underwater locomotion against gravity. By combining tunable wettability with robust photothermal performance, these MXene-LCE composites open new opportunities for designing and integrating stimuli-responsive materials in aquatic actuation systems.