Design of pure rolling line gear mechanisms for an arbitrary angle intersecting shafts was presented in this article. Based on the active design method of meshing line function for orthogonal shafts, three meshing types of conjugated tooth surfaces for an arbitrary angle intersecting shafts were discussed, including the parametric equations of different generatrix circles, the mathematical models of tooth surfaces, and central curves to be constructed, respectively. The validity of the active designed meshing line function was verified according to meshing equations, and the theoretical sliding rations were analyzed to prove pure rolling meshing. Then basic design parameters of pure rolling line gear mechanisms for the geometry design were determined, and the main structural parameters were obtained therefrom. Lastly, three groups of numerical examples were proposed according to mathematical models. Resin samples of line gears were processed by rapid prototyping technology and the kinematic performance of the pure rolling line gear mechanisms were validated. This paper laid the foundation of geometry and parameter design for pure rolling line gear mechanisms for an arbitrary angle intersecting shafts.