In this study, a detector is developed using deuterated L‐alanine doped triglycine sulfate (DLATGS) crystals capable of detecting circularly polarized light (CPL) and various polarization states. As a primary pyroelectric detection crystal, DLATGS has exhibited notable optical responses to both linearly and circularly polarized light during the tests, demonstrating a favorable polarization ratio of 3.86 and an anisotropic factor of 0.529. The research discovers the broad‐spectrum bulk photovoltaic (BPVE) characteristics in DLATGS, highlighting its potential for CPL detection. By integrating linear and circular bulk photovoltaic effect theories (LBPV and CBPV), the crystal's ability to differentiate between various polarization modes, including left‐/right‐handed polarized light, is confirmed. The BPVE and pyro‐phototronic coupling responses is characterized, laying a theoretical foundation for a rare pyroelectric effect‐based multifunctional polarization detector. The overall consistency of phenomena and theoretical framework bridges the gap between theoretical predictions and experimental validation. This work not only advances the understanding of DLATGS crystals but also sets the stage for further exploration into chiral materials and the development of TGS‐type crystals in future photoelectronic detectors.