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Poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a promising material because of its favorable electrical and mechanical properties, stability in ambient environments, and biocompatibility. It finds broad application in energy storage, flexible electronics, and bioelectronics. Additive manufacturing opens a plethora of new avenues to form and shape PEDOT:PSS, allowing for the rapid construction of customized geometries. However, there are difficulties in printing PEDOT:PSS while maintaining its attractive properties. A 3D printing method for PEDOT:PSS using a room‐temperature coagulation bath‐based direct ink writing technique is reported. This technique enables fabrication of PEDOT:PSS into parts that are of high resolution and high conductivity, while maintaining stable electrochemical properties. The coagulation bath can be further modified to improve the mechanical properties of the resultant printed part via a one‐step reaction. Furthermore, it is demonstrated that a simple post‐processing step allows the printed electrodes to strongly adhere to several substrates under aqueous conditions, broadening their use in bioelectronics. Employing 3D printing of PEDOT:PSS, a cortex‐wide neural interface is fabricated, and intracranial electrical stimulation and simultaneous optical monitoring of mice brain activity with wide field calcium imaging are demonstrated. This reported 3D‐printing technique eliminates the need for cumbersome experimental setups while offering desired material properties.