Hybrid organic–inorganic perovskite light‐emitting devices (LEDs) have recently shown the characteristic dynamical behavior of light‐emitting electrochemical cells (LECs), with intrinsic ionic migration creating an electric double layer and internal p‐i‐n structure and by accumulation of ions at interfaces. Therefore, the development of perovskite light‐emitting and photovoltaic devices based on the concepts of LEC operation attracts much attention and clarifies general physical processes in perovskites. Here, new directions that can further improve perovskite optoelectronic devices and extend their functionalities using additive mobile ions are overviewed: 1) enhancing single‐layer LECs with lithium additives for increased efficiency and longer lifetime; 2) facilitating ionic motion in three‐layer perovskite LECs to create dual‐functional devices, operating as both LEC and solar cells; and 3) creating truly ambipolar LEC devices with carbon nanotubes as stable electrodes that leverage ionic doping. Taken together, the use of these approaches provides a strategy to create efficient, stable, and bright LECs, which use advantages of both LED and LEC operation. It is discussed that how the LEC behavior in perovskite LEDs can be further improved to address the long‐term challenges in perovskite optoelectronics, such as stability, through approaches like ionically reconfigurable host/guest systems. [ABSTRACT FROM AUTHOR]