Cutting edge biomedical tools employ flexible optoelectronic devices combined with optogenetic mouse models providing high spatiotemporal modulation of specific brain activity. However, most applications were limited to activation of only one functional region using blue-light drivable channelrhodopsin. This thesis illustrates AlGaInP vertical light-emitting diodes (VLEDs) on flexible substrate for excitation of mouse motor cortex. Cell-sized chips effectively compress the conductive balls dispersed in anisotropic conductive film (ACF) resulting red-light emission with high optical power density. Selective operation of pulsed red-light from cell-sized flexible VLEDs (cf-VLEDs) induce mouse body movements and synchronized electromyogram (EMG) signals. Expression of chrimson, red-shifted channelrhodopsin, enables red-light excitation of detailed functional area of motor cortex. In addition, flexible electrocorticography (ECoG) electrode and its new insertion method beneath the skull facilitate large area neural signal analysis of mouse cortex in freely moving mice.