Homochiral metal–organic frameworks (HMOFs) have garnered considerable attention due to their extrachiral properties and broad application for chiral recognition. However, assembling a pair of high-quality chiral MOFs for sensing enantiomers precisely is a formidable challenge because of the complicated chiral environment and uncontrollable coordinated conditions. Herein, one pair of homochiral UiO-66 analogues, S-1 (L -AP@UiO-66-(COOH)2) and R-1 (D -AP@UiO-66-(COOH)2), are reported for chiral recognition. They were fabricated via a condensation reaction between the carboxyl groups of UiO-66-(COOH)2 and amino groups of L / D -amino propanol (L / D -AP). These novel fluorescent probes exhibited highly enantioselective fluorescence enhancement towards L / D -phenylalaninol (L / D -PA). For example, when S-1 and R-1 were treated with L -PA or D -PA, they displayed different fluorescence responses: the enantiomeric fluorescence enhancement ratio (ef) was 2.51 and 0.41 for S-1 and R-1 , respectively. Hence, a visible difference in fluorescence enhancement for L -PA and D -PA and excellent enantioselective behavior between S-1 and L -PA (or R-1 and D -PA) was displayed. Measurements of fluorescence lifetime, powder X-ray diffraction, molecular-dynamic simulations and Benesi–Hildebrand plots were employed to determine the observed high enantioselectivity for L / D -PA. In brief, we found that two post-modified HMOFs, S-1 and R-1 , were outstanding enantioselective sensors for detecting L -PA and D -PA. They had a prominent difference in ef and remarkable enantioselectivity factor α and ΔΔG based on steric hindrance and stereochemical difference. [ABSTRACT FROM AUTHOR]