(1 of 9)Planar integrated systems of micro-supercapacitors (MSCs) and sensors are of profound importance for 3C electronics, but usually appear poor in compatibility due to the complex connections of device units with multiple mono-functional materials. Herein, 2D hierarchical ordered dual-mesoporous polypyrrole/graphene (DM-PG) nanosheets are developed as bi-functional active materials for a novel prototype planar integrated system of MSC and NH 3 sensor. Owing to effective coupling of conductive graphene and highsensitive pseudocapacitive polypyrrole, well-defined dual-mesopores of ≈7 and ≈18 nm, hierarchical mesoporous network, and large surface area of 112 m 2 g −1 , the resultant DM-PG nanosheets exhibit extraordinary sensing response to NH 3 as low as 200 ppb, exceptional selectivity toward NH 3 that is much higher than other volatile organic compounds, and outstanding capacitance of 376 F g −1 at 1 mV s −1 for supercapacitors, simultaneously surpassing single-mesoporous and non-mesoporous counterparts. Importantly, the bi-functional DM-PG-based MSC-sensor integrated system represents rapid and stable response exposed to 10-40 ppm of NH 3 after only charging for 100 s, remarkable sensitivity of NH 3 detection that is close to DM-PG-based MSC-free sensor, impressive flexibility with ≈82% of initial response value even at 180°, and enhanced overall compatibility, thereby holding great promise for ultrathin, miniaturized, body-attachable, and portable detection of NH 3 .