Liquid crystalline‐based actuators containing azobenzene photoswitches have been used to demonstrate light‐responsive motion in soft actuator systems. Understanding the mechanical performance of these light‐responsive actuators as a function of the polymer chemistry as well as the nature and concentration of the photoswitches is crucial for developing advanced applications. A systematic study is presented here that clarifies the role of azobenzene photoswitches and the liquid crystalline networks in generating the desired photomechanical performance. Through measurement of photo stimulated mechanical behavior, in particular generated force and strain, a generalized set of guidelines concerning the appropriate subset of polymer chemistry and photoswitches required to achieve the desired performance for actuator design is derived. Light‐responsive motion has been demonstrated in soft actuator systems using liquid crystalline‐based actuators with azobenzene photoswitches. Understanding the mechanical performance of these light‐responsive actuators as a function of polymer chemistry and the concentration of photoswitches is critical for developing advanced applications. A systematic study that clarifies the role of azobenzene photoswitches and liquid crystalline networks in achieving the desired photomechanical performance is presented here.