Plants produce an array of different volatile organic compounds (VOCs) that have diverse eco-physiological functions and agricultural applications. Hence, the potential of VOCs as a natural and eco-friendly solution to increase crop productivity has garnered substantial attention. In particular, VOC-based pest management measures, such as Push–Pull, have been widely investigated in different cropping systems. However, our understanding of how the release and use of these VOCs impact agro-ecosystems beyond the targeted effects is still very limited. Therefore, studying the functions of plant VOCs from the perspective of pleiotropy may offer insights into optimizing and improving the effectiveness of VOC-based agronomic practices. Here, we discuss the current literature on the pleiotropic functions of plant VOCs, illustrate the underlying mechanism for their production and propose a systematic perspective for the usage of plant VOCs to enhance the sustainable management of crop health.