For the effective comminution and subsequent enrichment of mineral ores, comprehensive knowledge of their mineralogical and physical properties is required. Using an integrated methodology, this study evaluated samples of polymetallic Ni-Cu ore from Zapolyarnoe, Russia. Several analytical techniques were utilised, including optical microscopy, microindentation with Vickers geometry, the Point Load Test, and Mineral Liberation Analysis (MLA). The purpose of this study was to determine mineral associations, physical features, and enrichment during jaw crusher comminution. The acquired properties included the Point Load Strength Index, Vickers Hardness Number, and fracture toughness. The MLA method characterised seven fractions in terms of particle size distribution, degree of liberation, association, and modal mineralogy. Magnetite, pyrrhotite, pentlandite, and chalcopyrite were calculated in terms of wt% and their textural features. The enrichment of each ore phase in fractions with particle sizes smaller than 400 µm was determined. The influence of this enrichment was discovered to be correlated with various textural and structural parameters, such as intergrowth, grain size, and crack morphologies after indentations. In addition, the chromium content of magnetite contributed to an increase in the fracture toughness values. Despite the complexities involved, even limited samples of materials provide valuable insights into processing behaviour, emphasising the importance of considering mineralogical parameters in comminution studies.