In this study, LiNbO3 (LNO) thin films prepared by crystal ion slicing (CIS) technology have been used to fabricate pyroelectric infrared detectors. Crack free LNO film with single crystal structure have been prepared on a LNO holder substrate by CIS technology using He+ implantation and benzocyclobutene (BCB) bonding process. The surface roughness caused by the Gauss distribution of He+ has been decreased from 10.81 nm to 4.66 nm after Ar+ treatment. The pyroelectric coefficient of LNO thin film is 5 × 10−5C/m2·K measured by dynamic method, which is comparable to LNO bulk crystal materials. The Rv value of infrared device fabricated by LNO single crystal film was calculated to be 1.93 × 103 V/W at 5 Hz chopper frequency. Compared to normally used SiO2 bonding layer, the thermal isolation properties have been improved by BCB bonding material according to the thermal finite element analysis. The results demonstrated CIS technology using BCB bonding materials is a promising method to fabricate integrated pyroelectric devices.