The potential of cross-border regional cooperation development is important for evaluating the present and future capacity for regional development. Primorsky Krai (Russia) and Jilin (China) share borders and complementary advantages. China and Russia have growing intention to strengthen cooperation, with geopolitical considerations. This study constructs a regional development potential assessment index system from the perspective of cross-border cooperation, and it establishes a multilayer cross-border regional development potential assessment (RDPA) model with three layers: target, factor, and indicator. By coupling four modules (economic, social, transportation, and resource environment), this study builds a development potential value system. The results illustrate that Primorsky Krai and Jilin have potential for cross-border cooperative development. The results reveal that Primorsky Krai has comparative advantages in port logistics, agriculture, fishery, and mining, which are all complementary to Jilin. These are important directions for cross-border international cooperation. Additionally, this study provides suggestions on decision-making and strategy consultation for the international cooperation between Jilin and Primorsky Krai and creates references for the study of cross-border cooperation opportunities and challenges for other neighboring regions around the world.