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.