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Bioelectrocatalytic systems are based on biological entities, such as enzymes, whole cells, parts of cells or tissues, which catalyse electrochemical processes that involve the interaction between chemical change and electrical energy. In all cases, biocatalysis is implemented by enzymes, isolated or residing inside cells or part of cells. Electron transfer (ET) phenomena, within the protein molecules and between biological redox systems and electronics, enable the development of various bioelectrocatalytic systems, which can be used both for fundamental investigations of enzymatic biological processes by electrochemical methods and for applied purposes, such as power generation, bioremediation, chemical synthesis and biosensing. Electrical communication between the biocatalyst’s redox centre and an electrode is essential for the functioning of the system. This can be established using two main mechanisms: indirect ET and direct ET. The efficiency of the ET influences important parameters such as the turnover rate of the biocatalyst, the generated current density and partially the stability of the system, which in their turn determine response time, sensitivity, detection limit and operational stability of biosensing devices or the power densities and current output of biofuel cells, and hence should be carefully considered when designing bioelectrocatalytic systems. This thesis focuses on approaches that facilitate ET in bioelectrocatalytic systems based on indirect and direct ET mechanisms. Both fundamental aspects of ET in bioelectrocatalytic systems and applications of such systems for biosensing and power generation are considered. First, a new hydrophobic mediator for oxidases – unsubstituted phenothiazine and its improved ET properties in comparison with commonly used mediators are discussed. Application of the mediator in electrochemical biosensors is demonstrated by glucose, lactate and cholesterol sensing. Utilisation of mediated biocatalytic cholesterol oxidation, as the anodic reaction for the construction of a biofuel cell acting as a power supply and an analytical device at the same time, is investigated to deliver a selfpowered biosensor. Also the enhancement of mediated bioelectrocatalysis by employment of microelectrodes as a transducer is examined. The effect of surface roughness on the current response of the microelectrodes under conditions of convergent diffusion is considered. The applicability of the laccase-based system for total phenol analysis of weakly supported water is demonstrated. Finally, a new electrochemical approach derived from collision-based electrochemistry applicable for examination of the ET process of a single enzyme molecule is described. All together, the results presented in this thesis contribute to the solution of the ‘electronic coupling problem’, arising when interfacing biomolecules with electronics and limiting the performance of bioelectrocatalytic systems in specific applications. The developed methods to facilitate ET will hopefully promote future biosensing devices and biofuel cells. I believe the new approach for investigation of ET processes at a single enzyme molecule will complement existing single molecule techniques, giving further insights into enzymatic ET mechanisms at the molecular level and filling the gap between fundamental understanding of biocatalytic processes and their potential for bioenergy production

Facilitating electron transfer in bioelectrocatalytic systems