The exploration of neural circuitry is essential for understanding the computational mechanisms and physiology of the brain. Despite significant advances in materials and fabrication techniques, controlling neuronal connectivity and response in three dimensions continues to present a formidable challenge. Here, we present a method for engineering the growth of three-dimensional (3D) neural circuits with the capability for optical stimulation. We fabricated bioactive interfaces by melt electrospinning writing (MEW) of 3D printed polycaprolactone (PCL) scaffolds followed by coating with titanium carbide (Ti3C2Tx MXene). Beyond enhancing hydrophilicity, cell adhesion, and electrical conductivity, the Ti3C2Tx MXene coating enabled optocapacitance-based neuronal stimulation due to illumination-induced local temperature increases. This work presents a strategy for additive manufacturing of neural tissues with optical control for functional tissue engineering and neural circuit computation.