In this paper, a novel multipiece actuator configuration is first proposed. This configuration exhibits several advantages over the existing ones, such as: (1) the ability to overcome the deficiency of one-way actuation of PbLaZrTi (PLZT) actuators and (2) all of the actuators in this configuration being placed on the inner surfaces of a thin cylindrical shell and the removal of extra electrical wires between the end surfaces of the actuators. A new index of modal control factors is defined, and an optimization method for allocating actuator is proposed. By using the proposed method, the PLZT actuators can be located in an optimum position. Moreover, in view of the nonlinear and time-variant characteristics of photostrictive actuators, a self-organizing fuzzy sliding mode control (SOFSMC) method is established to attenuate multimodal vibration of photo-electric laminated thin cylindrical shells. A multilevel sliding mode surface is defined as fuzzy input and the SOFSMC method is used to infer the applied light intensity. Its control rule bank can be developed and adjusted continuously via online learning. In addition, using fuzzy sliding mode, the chatter inherent in conventional sliding mode control is therefore managed effectively while ensuring sliding mode behavior. Case studies demonstrate that the proposed approach can efficiently suppress multimodal vibration of photo-electric laminated thin cylindrical shells. It is also founded that SOFSMC can achieve better control effect than fuzzy neural network control (FNNC).