Two-ion crystals constitute a platform for investigations of quantum nature that can be extended to any ion species or charged particle provided one of the ions in the crystal can be directly laser cooled and manipulated with laser radiation. This paper presents the formation of two-ion crystals for quantum metrology in a 7-tesla open-ring Penning trap. 40 Ca + ions are produced either internally by photoionization or externally in a (Paul-trap) source, transported through the strong magnetic field gradient of the superconducting solenoid, and captured in-flight with a mean kinetic energy of a few electronvolts with respect to the minimum of the Penning-trap potential well. Laser cooling of the two-ion crystal in a strong magnetic field towards reaching the quantum regime is also presented, with particular emphasis on the cooling of the radial modes.