High-performance X-ray detectors are usually based on single crystals, due to the long-range ordering and hence outstanding electronic properties. On the other hand, bulk heterojunctions (BHJs) that can effectively enhance photogenerated exciton dissociation are widely used for photodetectors. The benefits of both spur investigation into how to combine these two strategies to enhance X-ray detection. Here, TiO 2 networks are incorporated into PbI 2 crystals to form interpenetrating type II heterojunctions, namely BHJs. These BHJs exhibit long-range ordering in molecular packing similar to that of single crystals. Compared with single crystals, the long-range ordered BHJs facilitate the separation of photogenerated electrons and holes to inhibit recombination, extend the mobility lifetime product by 6.4 times, and consequently improve X-ray sensitivity by 5.8 times. Hence, this work provides a new strategy using gel-grown crystals to fabricate highperformance X-ray detectors as well as a new platform for studying the behavior of X-raygenerated carriers in BHJs with long-range ordering.