Over the past decade, conductive hydrogels have received great attention as tissue-interfacing electrodes due to their soft and tissue-like mechanical properties. However, a trade-off between robust tissue-like mechanical properties and good electrical properties has prevented the fabrication of a tough, highly conductive hydrogel and limited its use in bioelectronics. Here, we report a synthetic method for the realization of highly conductive and mechanically tough hydrogels with tissue-like modulus. We employed a template-directed assembly method, enabling the arrangement of a disorder-free, highly-conductive nanofibrous conductive network inside a highly stretchable, hydrated network. The resultant hydrogel exhibits ideal electrical and mechanical properties as a tissue-interfacing material. Furthermore, it can provide tough adhesion (800 J/m ) with diverse dynamic wet tissue after chemical activation. This hydrogel enables suture-free and adhesive-free, high-performance hydrogel bioelectronics. We successfully demonstrated ultra-low voltage neuromodulation and high-quality epicardial electrocardiogram (ECG) signal recording based on in vivo animal models. This template-directed assembly method provides a platform for hydrogel interfaces for various bioelectronic applications.