Nitrides, carbides, and borides of transition metals are an attractive class of hard materials. Our recent preliminary explorations of the binary chemical compounds indicated that chromium-based materials are among the hardest transition metal compounds. Motivated by this, here we explore in detail the binary Cr-B, Cr-C, and Cr-N systems using global optimization techniques. Calculated enthalpy of formation and hardness of predicted materials were used for Pareto optimization to define the hardest materials with the lowest energy. Our calculations recover all numerous known stable compounds (except CrC with its large unit cell) and discover a novel stable phase Pmn2-CrC. We resolve the structure of CrN and find it to be of anti-CaCl type (space group Pnnm). Many of these phases possess remarkable hardness, but only CrB is superhard (Vickers hardness 48 GPa). Among chromium compounds, borides generally possess the highest hardnesses and greatest stability. Under pressure, we predict stabilization of a layered TMDC-like phase of CrN, a WC-type phase of CrN, and a new compound CrN. Nitrogen-rich chromium nitride CrN is a high-energy-density material featuring polymeric nitrogen chains. In the presence of metal atoms (e.g., Cr), polymerization of nitrogen takes place at much lower pressures; CrN becomes stable at ∼15 GPa (cf. 110 GPa for synthesis of pure polymeric nitrogen).