Memristive systems emerge as strong candidates for the implementation of Resistive Random Access Memories (RRAM) and neuromorphic computing devices, as they can mimic the electrical analog behavior or biological synapses. In addition, complementary functionalities such as memcapacitance could significantly improve the performance of bio-inspired devices in key issues such as energy consumption. However, the physics of mem-systems is not fully understood so far, hampering their large-scale implementation in devices. Perovskites that undergo topotactic transitions and redox reactions show improved performance as mem-systems, compared to standard perovskites. In this paper we analyze different strategies to optimize the multi-mem behavior (memristive and memcapacitive) of topotactic redox La 1/2 Sr 1/2 Mn 1/2 Co 1/2 O3−x (LSMCO) films grown on Nb:SrTiO3 (NSTO). We explored devices with different crystallinity (from amorphous to epitaxial LSMCO), out-of-plane orientation (( 001) and ( 110)) and stimulated either with voltage or current pulses. We found that an optimum memory response is found for epitaxial (110) LSMCO stimulated with current pulses. Under these conditions, the system efficiently exchanges oxygen with the environment minimizing, at the same time, self-heating effects that trigger nanostructural and chemical changes which could affect the device integrity and performance. Our work contributes to pave the way for the integration of LSMCO-based devices in cross-bar arrays, in order to exploit their memristive and memcapacitive properties for the development of neuromorphic or in-memory computing devices