The maximum current flowed with zero resistance, referred to the critical current density, is desired to be sufficiently large in order to apply superconducting wire rods and electromagnets to various devices. Although the critical current density can be enhanced by introduction of non‐superconducting impurities, the transition temperature would become diminished in such a case. Here, we report modulation of a critical current density in heavily boron‐doped diamonds (BDDs) by changing the surface‐termination without introducing any impurity. The surface of a BDD was changed between hydrogen‐ and oxygen‐termination. As a result, the critical current density could be modulated in a reversible manner between the hydrogen‐ and oxygen‐terminated diamonds with maintenance of the superconducting transition temperature. This is because the volume fractions of the superconducting phases were modulated by surface modification.