The response of U-6-depleted Cs2LiYCl6 (CLYC) to high-energy neutrons has been investigated using a pair of 1 in. x 1 in. crystals. These are the first two detectors of their kind, which will comprise a 16-element array for studies in fast neutron spectroscopy. Their thermal neutron response has been compared with standard CLYC crystals with a Li-6 enrichment of 95%, demonstrating excellent suppression of the overwhelming thermal neutron background. The response to mono-energetic neutrons over a range of 0.5 to 20 MeV was tested. From this, the response function, energy resolution, and pulse-shape discrimination up to 20 MeV were characterized. Detailed Monte Carlo investigations with MCNPX have been used to show that the dominant reaction mechanisms contributing to the observed response are Cl-35(n,p) and Cl-35(n,alpha). Preliminary investigations have also demonstrated the possibility for separating events from these two reactions. (C) 2014 Elsevier B.V. All rights reserved.