Bioelectronics is the integration of biology with microelectronic devices. The combination of biology with microelectronics can potentially provide new systems for electricity generation, chemical production, environmental sensing, health diagnosis, disease treatment, a greater understanding of biology, and biomimetic materials and devices. Microelectronic devices are traditionally based on hard materials and rely on electronic signals while biology uses soft materials and a combination of ionic, molecular, and electron transfer for communication and signaling. Therefore, producing functional devices through the integration of these two fields requires addressing fundamental challenges in material properties, forms of signaling and communication, biocompatibility, and structures across various length scales. This thesis focuses on the development of functional electrode surface and polymeric networks and the fabrication of novel microbial bioelectronic devices to enhance bidirectional electrical and molecular communication. To bridge the gap between the biology and electronic worlds and improve the communication between them, this thesis pinpoints the solution for three key challenges including stable microbial adhesion, microbial patterning, and signal amplification. Prior research has developed and engineered two or three-dimensional biology-material interface layers to achieve dense microbial encapsulation, efficient electron transfer, and better nutrient and waste transport. However, we still lack electrode modification approaches that can be deposited easily and cheaply on an electrode surface, are amenable to patterning, and produce a significant enhancement to current densities. This thesis shows a solution-processable conductive polymer thin film that readily modifies the electrodes for diverse bioelectronics that take advantage of the high current density and microbial patterning on a surface. Furthermore, the integration of novel bioelectronic devices, specifically organic electrochemical transistor (OECT), with the microbes and enzymes demonstrates the power of amplifying minuscule electronic and ionic signals from biological entities compared to traditional three-electrode electrochemical systems. This research will lead to robust devices for monitoring enzymatic and microbial activities and benefit the material design and development of microbial bioelectronics for a broad class of sensitive and responsive biosensors.