The invention provides a nanomaterial microstructure 2D/3D printing device. The device comprises an ink supply system, an ultrasonic three-way mixing pipe, and a three-shaft device with a printing head automatic adjusting function; a high-precision laser microdistance measuring head in the three-shaft device is mounted on the side surface of a printing head fixer; and a temperature controllable heating plate is mounted below the printing head fixer. Meanwhile, the invention provides an operation method of the nanomaterial microstructure 2D/3D printing device. The nanomaterial microstructure 2D/3D printing device has the following beneficial effects: the device uses a microdistance automatic adjusting mode for automatical identification to achieve the precision of 1 micron in the whole printing process to guarantee seamless contact with a baseplate and seamless connection between layers. The ink outlet quantity of a micro controllable ink supply system is controlled to 0.001-0.1 mL. Double printing heads are adjusted in a range of 10 microns to 5 cm, and are combined with double ink supply devices to realize alternate use between double printing heads and single printing head to print out different microstructures; and ultrasonic pipes are combined to uniformly mix different nanometer ink to improve the 2D/3D printing quality.