Green diopside is currently popular in the jewelry market due to its attractive color and excellent transparency. Gem-quality diopsides are mainly sourced from Pakistan, Italy, Russia, and other places. The color, geographic origin, and formation mechanism are the main factors affecting the value of gemstones, which can be determined by examining their gemology and composition characteristics. This study systematically characterizes the standard gemology of green diopsides from Pakistan and Russia and compares them with the blue diopsides produced within the skarn process and the diopsides from the nearby region in Russia from previous studies by gemological microscopy, spectral testing (infrared, Raman and ultraviolet-visible spectroscopy), and chemical analyses (electron probe and laser ablation inductively coupled plasma mass spectrometry). The results show that the spectral characteristics and phase composition of the green diopside samples from Pakistan and Russia have excellent uniformity and similarity. The high Cr, Fe, V, and Ni contents are the reasons why they appear as green. Meanwhile, the elemental characteristics of the diopside are effective tools for distinguishing different origins of different diopsides. The Russian green diopsides have higher contents of Sr, Sc, Zr, and rare earth elements (REE), indicating that they are related to alkaline ultrabasic rocks, and the source of the diopside sample from Pakistan is metamorphic rock.