Chiral Metal‐Organic Frameworks (CMOFs) are a rapidly growing field reflecting their potential as selective and sensitive chemical sensors for chiral analytes. The highly tuneable nature of CMOFs enables the size, shape, and non‐covalent interactions to be optimised towards specific analytes to engender strong intermolecular interactions and sensing responses. While CMOFs as chiral chemical sensor devices have been explored with electrochemical methods including differential pulse voltammetry (DPV), bipolar and chemiresistive sensing techniques, the CMOFs as chiral chemical sensors using spectroscopic methods has received significantly less attention. This review examines the synthesis of CMOFs for chemical sensors with spectroscopic methods such as photoluminescence, circular dichroism, and solid‐state nuclear magnetic resonance with a view towards their incorporation into chemical sensor devices. Future directions of the field are highlighted for the generation of functional devices.