Thallium bromide (TlBr) is a semiconductor material and, simultaneously, a good Cerenkov radiator. The performance of a TlBr detector that integrates two different readouts, the charge induction readout and the detection of Cerenkov light, was evaluated. A TlBr detector with dimensions of 4 × 4 × 5 mm3, with a monolithic cathode and an anode segmented into strips, was manufactured. One of the bare and polished 4 × 4 mm2 faces of the detector was coupled to a silicon photomultiplier (SiPM) to read out the Cerenkov light. Simultaneous timing and energy resolutions of <400 ps full width at half maximum (FWHM) and ~8.5% at 511 keV were measured using the Cerenkov detection and charge induction readouts, respectively. A coincidence time resolution of 330 ps was obtained when selecting Cerenkov events with amplitudes above 70 mV. The combination of both readouts showed the potential to resolve the depth-of-interaction (DOI) positioning, based on the improvement of energy resolution when selecting events with similar electron drift times. This manuscript sets the stage for a new family of semiconductor detectors that combine charge induction readout with the Cerenkov light detection. Such detectors can provide, simultaneously, outstanding timing, energy, and spatial resolution, and will be an excellent fit for applications that require the detection of high-energy gamma photons with high timing accuracy, such as time-of-flight positron emission tomography (TOF-PET) and prompt gamma imaging (PGI) to assess the particle range in hadron therapy.