Untethered intelligent soft robots capable of autonomous, continuous, directional, and fast movements under external stimuli have great potential in environmental, industrial, military, and medical fields. This paper used an unconventional dual-flow filtration method to prepare a laterally heterogeneous MXene-NiFe2O4/Polycarbonate bilayer membrane. Based on this, a one-piece untethered soft crawling robot with multi-stimulus synergistic control is developed, which can achieve relatively fast crawling up to 3.77 mm/s and directional turning locomotion. In addition, a cross-shaped robot that can realize biaxial flipping locomotion is developed by using the inverse snapping property of the polycarbonate films under light and humidity excitation. The preparation method has also been extended to unconventional multi-flow filtration and applied to bionic flowers and asymmetric grippers with biological gradients. This work provides an effective way for designing soft crawling robots with fast actuation performance and adjustable trajectories that can be used in areas such as bionic soft robots and biomedical systems.