A major goal of MOF research is to design its structure and function for specific applications. In this study, we have successfully synthesized two In-MOFs (In-MOF1 and In-MOF2). The structures of the two kinds of MOFs were characterized, both MOFs contain 9-connected trinuclear indium cluster units, which is rare in the reported In-MOF structures. In-MOF1 demonstrated a three-dimensional network configuration based on the [In3(μ3–O)(CO2)6N2O] SBUs, In-MOF2 demonstrated a three-dimensional network framework based on the [In3(μ3–O)(CO2)6N3] SBUs. Both In-MOF1 and In-MOF2 showed high selective and sensitive for fluorescence detection toward Fe3+ ion in water. In addition, the gas adsorption experiments show that In-MOF1 has the ability to selectively adsorb C2H2 and CO2 over CH4.