The synthesis of solution-processed two-dimens i o n a l( 2 D ) l a y e r e d o r g a n o h a l i d e (CH 3 (CH 2 ) 3 NH 3 ) 2 (CH 3 NH 3 ) n−1 Pb n I 3n+1 (n = 2, 3, and 4) perovskites is presented, where inkjet printing was used to fabricate heterostructure flexible photodetector (PD) devices on polyimide (PI) substrates. Inks for the n = 4 formulation were developed to inkjet-print PD devices that were photoresponsive to broadband incoming radiation in the visible regime, where the peak photoresponsivity R was calculated to be ∼0.17 A/W, which is higher compared to prior reports, while the detectivity D was measured to be ∼3.7 × 10 12 Jones at a low light intensity F ≈ 0.6 mW/cm 2 . The ON/OFF ratio was also high (∼2.3 × 10 3 ), while the response time τ on the rising and falling edges was measured to be τ rise ≈ 24 ms and τ fall ≈ 65 ms, respectively. Our strain-dependent measurements, conducted here for the first time for inkjetprinted perovskite PDs, revealed that the I p decreased by only ∼27% with bending (radius of curvature of ∼0.262 cm −1 ). This work demonstrates the tremendous potential of the inkjet-printed, composition-tunable, organohalide 2D perovskite heterostructures for high-performance PDs, where the techniques are readily translatable toward flexible solar cell platforms as well.