devices in various fields, such as sensing and energy storage/conversion devices. Microfluidic technologies enable miniaturization and integration of various reaction processes and technologies into on-chip devices. [1,2] In traditional microfluidic systems, microfluidic channels are constructed by molding, photolithography, or etching glass, silicon or polymer substrates. [3][4][5] These substrates are rigid materials with high cost, making the systems less feasible for constructing flexible devices, especially single-use devices. Moreover, the flow within microfluidic channels is usually controlled by pumps, which inevitably increases the total cost of the system, thus making it difficult to miniaturize the whole device. [6,7] Compared with conventional microfluidic systems, paper emerges as an attractive microfluidic substrate. Paper is an inexpensive and environmentally friendly material with high flexibility. The hierarchical porous structure of paper with dimensions of tens to hundreds of micrometers is originated from the randomly interconnected cellulose fibers. [8] This structure enables liquid to flow spontaneously by capillarity, which eliminates the use of pumps. [9,10] Based on the wax printing and origami techniques, microfluidic channels can be precisely created on paper in various configurations, providing a feasible platform for the design and fabrication of a broad range of miniaturized electrochemical devices toward practical applications. [11][12][13][14] On the one hand, paper-based microfluidic technique has been widely used to develop electrochemical sensing devices in the fields of medical diagnosis, food safety analysis, environmental monitoring. [15][16][17][18][19][20] On the other hand, many types of portable and disposable energy devices (e.g., primary batteries, fuel cells, bio-batteries, metal-air batteries) are also designed and fabricated based on the paper-based microfluidic system. [21][22][23][24][25][26] Flow regulating is one of the key points in fabricating microfluidic electrochemical devices since the flow behavior of the liquid electrolyte can significantly influence the device performance. In conventional microfluidic systems, the flow dynamics can be easily controlled by pumps. While in paper-based microfluidic systems, the flow behavior can be manipulated by constructing paper channel with various structures. [27][28][29] In our previous work regarding the paper-based microfluidic fuel cell, we found that the microstructure of Paper-based microfluidics emerges as an innovative platform for constructing miniaturized electrochemical devices, which mainly benefit from the spontaneous capillary action of paper. Nevertheless, the capillary-driven flow dynamics on paper are determined exclusively by the intrinsic properties of paper and fluidics, thus lacking the controllability that conventional pump-based microfluidics can provide. Herein, an approach to regulating the capillary flow on paper is introduced by conjugating the outlets of microfluidic channels with a photothe...