Terahertz (THz) detection technology is getting increasing attention from scientists and industries alike due to its superiority in imaging, communication, and defense. Unfortunately, the detection of THz electromagnetic waves under room temperature requires a complicated device architecture design or additional cryogenic cooling units, which increase the cost and complexity of devices, subsequently imposing an impediment in its universal application. In this work, THz detectors operated under room temperature are designed based on the thermoelectric effect with MAPbI3 single crystals (SCs) as active layers. With solution-processed molecular growth engineering, the anti-reflection 2D perovskite layers were constructed on SCs' surfaces to suppress THz reflection loss. Simultaneously, by finely regulating the main carrier types and the direction of the applied bias across the inclined energy level, the thermoelectric effect is further promoted. As a result, THz-induced ΔT in MAPbI3 SCs reaches 4.6 °C, while the enhancement in the bolometric and photothermoelectric effects reach ∼4.8 times and ∼16.9 times, respectively. Finally, the devices achieve responsivity of 88.8 μA W-1 at 0.1 THz under 60 V cm-1, noise equivalent power (NEP) less than 2.16 × 10-9 W Hz-1/2, and specific detectivity (D*) of 1.5 × 108 Jones, which even surpasses the performance of state-of-the-art graphene-based room-temperature THz thermoelectric devices. More importantly, proof-of-concept imaging gives direct evidence of perovskite-based THz sensing in practical applications.