© 2015 American Chemical Society. Organometallic halide perovskites are a class of solution-processed semiconductors exhibiting remarkable optoelectronic properties. They have seen rapid strides toward enabling efficient third-generation solar cell technologies. Here, we report the first material-tailoring of TiO2/perovskite/spiro-OMeTAD junction-based photodiodes toward applications in photodetection, a field in need of fast, sensitive, low-cost, spectrally tunable materials that offer facile integration across a broad range of substrates. We report photodetection that exhibits 1 μs temporal response, and we showcase stable operation in the detection of over 7 billion transient light pulses through a continuous pulsed-illumination period. The perovskite diode photodetector has a peak responsivity approaching 0.4 A W^-1 at 600 nm wavelength, which is superior to red light detection in crystalline silicon photodiodes used in commercial image sensors. Only by developing a composite Al2O3/PCBM front contact interface layer were we able to stabilize device operation in air, reduce dark current, and enhance the responsivity in the low-bias regime to achieve an experimentally measured specific detectivity of 10¹² Jones.