This paper implements the design of a set of LIBS-Raman test systems in a laboratory environment. Based on the system’s LIBS and Raman spectroscopy techniques, it is used to verify the comprehensive detection capabilities of mineral samples in the Martian simulated environment. This system uses the Cassegrain telescope structure for long-range LIBS excitation and the bypass reflection optical path for Raman spectrum excitation. The wavelengths of excitation lasers are 1 064 and 532 nm, respectively. The Cassegrain telescope was then used to collect both spectra. In order to fully simulate the physical conditions of the minerals on the surface of Mars, we have designed a set of gas cavities. By placing samples in the gas chamber, the conditions on the surface of Mars can be simulated to the greatest extent. In order to verify the ability of this LIBS-Raman instrument to analyze Mars minerals, we performed experimental analysis using 8 typical samples (malachite, azurite, realgar, orpiment, aragonite, calcite, anhydrite and gypsum). There are huge differences in elements and molecules in these samples, among which malachite and azurite have molecules with different valence states and atomic ratios; the number of atoms of realgar and orpiment molecules is different; aragonite and calcite have the same molecular formula, but their crystal structures are significantly different; the difference between anhydrite and gypsum mineral is reflected in the presence or absence of crystal water in its molecules. These differences were studied using LIBS and Raman techniques to verify the effectiveness of using this combined instrument to analyze mineral types and components under Martian conditions, and to study the advantages and disadvantages of LIBS and Raman techniques in the analysis of material composition. Experimental results show that the system can effectively analyze mineral species and composition under Martian conditions. This comparative experiment also verified that LIBS could quickly distinguish element types in the analysis of specific mineral elemental composition in Martian material, but there are obvious limitations for molecular information detection; Raman technology can compensate for this limitation to a certain extent. The combination of the two will effectively improve the recognition efficiency of minerals with different molecular composition and structure under extreme conditions. The successful verification of the system can complement the further Mars exploration program and help the laboratory establish a valuable database.