This study investigates how long‐term partners can establish a successful supply chain collaboration to accrue relationship benefits. Informed by the relational view, we identify governance and resource sharing as key mechanisms to create relationship benefits in supply chain relationships. We draw on the ambidexterity perspective to suggest that long‐term relationships require governance ambidexterity and resource‐sharing ambidexterity to handle new problems emerging in the future while successfully managing current problems, or to have a duality of short-and long‐term orientation. We also draw on the alignment perspective to suggest that governance ambidexterity mechanisms and resource‐sharing ambidexterity mechanisms need to be aligned. We develop a research model that explains the influence of (1) alignment/misalignment of two governance ambidexterity mechanisms (incentives and goals) on one resource‐sharing ambidexterity mechanism (knowledge sharing) and (2) alignment/misalignment of each of these governance ambidexterity mechanisms (incentives and goals) with resource sharing (knowledge sharing) ambidexterity on relationship benefits. The data for our empirical study were collected from 238 customers of a leading logistics vendor firm. A polynomial regression and response surface approach was employed to test our model. The results were supportive of our model and suggest that establishing and aligning governance ambidexterity mechanisms and resource‐sharing ambidexterity mechanisms enable firms to generate relationship benefits from supply chain relationships.