In the present work, two of the most typical frustrated spin systems—triangular lattice antiferromagnets and edge-shared chain magnets—have systematically been investigated. Despite the crystallographic simplicity of target systems, rich magnetoelectric responses are ubiquitously observed. The current results published here offer a useful guideline in the search for new materials with unique magnetoelectric functions, and also provide an important basis for a deeper understanding of magnetoelectric phenomena in more complex systems.