The sensors of taste and odor play important roles of recognition as well as reception. In our research, the taste and odor sensing capabilities were based on the photoluminescence (PL) responses of luminescent metal-organic frameworks (MOFs). For the sensing of taste, [In(OH)(bdc)]n (bdc = 1,4-benzenedicarboxylate) and [Tb(btc)] (MOF-76, btc = benzene-1,3,5-tricarboxylate), were tested on aqueous solutions of five basic tastants such as sucrose (sweet), caffeine (bitter), citric acid (sour), sodium chloride (salty) and monosodium glutamate (umami). The photoluminescence (PL) responses of polyacrylic acid-chelated [In(OH)bdc]n and lanthanide Tb(btc) were used to demonstrate the applicability of MOF-based biomimetic tongue through: (1) identification of five tastes: sweet, bitter, sour, salty and umami, by 3-D PCA (principle component analysis) to distinguish the corresponding tastants, (2) quantification of the strength of five tastes determined by the relationships between the PL intensity and the τ scale of taste. For the sensing of odor, [In(OH)(bdc)]n and [Zn4O(bdc)3] (MOF-5) were exposed to the odorants such as cumin, cinnamon, vanillin, p-xylene, m-xylene, o-xylene, water, and ethanol. Similarly, the MOF-based biomimetic nose could distinguish the odors of the analytes based on a pattern recognition method (i.e., principal component analysis) constructed by the 2-D map of PL emission responses.