The ability of octocorals and stony corals to deposit calcium carbonate (CaCO3) has contributed to their ecological success. Whereas stony corals possess a homogeneous aragonite skeleton, octocorals have developed distinct skeletal structures composed of different CaCO3 polymorphs and a skeletal organic matrix. Nevertheless, the molecular basis of skeletal structure formation in octocorals remains inadequately understood. Here, we sequenced the genomes and skeletal proteomes of two calcite-forming octocorals, namely Paragorgia papillata and Chrysogorgia sp. The assembled genomes sizes were 618.13 Mb and 781.04 Mb for P. papillata and Chrysogorgia sp., respectively, with contig N50s of 2.67 Mb and 2.61 Mb. Comparative genomic analyses identified 162 and 285 significantly expanded gene families in the genomes of P. papillata and Chrysogorgia sp., respectively, which are primarily associated with biomineralization and immune response. Furthermore, comparative analyses of skeletal proteomes demonstrated that corals with different CaCO3 polymorphs share a fundamental toolkit comprising cadherin, von Willebrand factor type A, and carbonic anhydrase domains for calcified skeleton deposition. In contrast, collagen is abundant in the calcite-forming octocoral skeletons but occurs rarely in aragonitic stony corals. Additionally, certain collagens have developed domains related to matrix adhesion and immunity, which may confer novel genetic functions in octocoral calcification. These findings enhance our understanding of the diverse forms of coral biomineralization processes and offer preliminary insights into the formation and evolution of the octocoral skeleton.