The dual-mode elpasolite scintillation material CLLBC (Cs2LiLaBr4.8Cl1.2:Ce) is capable of measuring both𝛾-rays and neutrons. The neutron detection capability spans from thermal energies up to about 10 MeV,making these detectors attractive options for studying prompt fission neutron spectra (PFNS). In this work, acomprehensive characterization of CLLBC detectors is performed. Three CLLBC detectors were characterized,in addition to three LaBr3:Ce and two LaBr3:Ce,Sr for comparison. For the best-performing CLLBC detector,the results indicate an energy resolution of 3.7% at 𝐸𝛾 = 662 keV and an intrinsic timing resolution of1.2 ns (FWHM) above 𝐸𝛾 = 1 MeV using 60Co. A 𝛾-neutron separation figure-of-merit of 2.7 is obtainedby means of pulse-shape discrimination. Tagged neutron time-of-flight measurements were conducted usinga 241Am9Be neutron source, by coincident detection of the 4.44 MeV 𝛾-ray and the neutron, to determinethe intrinsic neutron detection efficiency between 2–6 MeV. Neutron detection efficiencies of about 0.2% forthe 6Li(n,t)4He reaction and 1% for three types of (n,n′) reactions were obtained. Two of three investigatedCLLBC detectors exhibit an energy peak asymmetry, resulting in worse performance, indicating scintillatorquality issues and motivating further investigation. Future studies are anticipated using the 252Cf(sf) promptfission neutron spectrum to determine neutron efficiencies for a wider range of neutron energies. Althoughobserved in a previous study, neutron detection via 35Cl(n,p)35S was not identified in this work but is plannedto be determined using quasi-monoenergetic neutrons generated at the JRC MONNET facility.