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Fabrication of hydrogel composites embedded with aligned 1D nanoparticles has shown substantial growth over the past 5 years. Direct ink printing technology (DIW) has been used in this work to create the alignment of the 1D nanoparticles due to the shear gradient of the pseudoplastic precursor (2-hydroxyethyl methacrylate (HEMA) with thickening agents). Orderly distributed 1D particles constructing anisotropic nanostructures endow the hydrogel composite with unique mechanical, electric, or electromechanical coupling properties. Quasi-static uniaxial tensile test, electric resistivity, and piezoresistivity measurements have been conducted for investigating the mechanical, electric, and electromechanical coupling properties of the hydrogel composites, respectively. Based on the experimental results, it can be speculated that the developed printing process is able to fabricate hydrogel composites with programmable anisotropic mechanical, electric, and electromechanical properties. The products pumped out from this work have the potential of being substrates for soft devices and may have a great impact on the fields of flexible bioelectronics.