The design of mobile X-ray C-arm equipment with image tomography and surgical guidance capabilities involves the retrieval of repeatable gantry positioning in three-dimensional space. Geometry misrepresentations can cause degradation of the reconstruction results with the appearance of blurred edges, image artifacts, and even false structures. It may also amplify surgical instrument tracking errors leading to improper implant placement. In our prior publications we have proposed a C-arm 3D positioner calibration method comprising separate intrinsic and extrinsic geometry calibration steps. Following this approach, in the present paper, we extend the intrinsic geometry calibration of C-gantry beyond angular positions in the orbital plane into angular positions on a unit sphere of isocentric rotation. Our method makes deployment of markerless interventional tool guidance with use of high-resolution fluoro images and electromagnetic tracking feasible at any angular position of the tube-detector assembly. Variations of the intrinsic parameters associated with C-arm motion are measured off-line as functions of orbital and lateral angles. The proposed calibration procedure provides better accuracy, and prevents unnecessary workflow steps for surgical navigation applications. With a slight modification, the Misalignment phantom, a tool for intrinsic geometry calibration, is also utilized to obtain an accurate 'image-to-sensor' mapping. We show simulation results, image quality and navigation accuracy estimates, and feasibility data acquired with the prototype system. The experimental results show the potential of high-resolution CT imaging (voxel size below 0.5 mm) and confident navigation in an interventional surgery setting with a mobile C-arm.