The synthesis of thiophene-pyrrole hybrid polymers has become of increased interest due to their potential in a wide range of applications, from optoelectronics to biodevices. While the extended application of these materials in optoelectronics or photovoltaics has been previously addressed, a comprehensive account on their potential for application in sensorics has not been reported so far. The main advantages derived from their application are related to facility in synthesis and stable electrochemical behavior with the added benefit of tailor-made functionality. As it has become clear that the ultimate goal in electrochemical sensing is the preparation of a conducting platform that not only exhibits satisfactory conductivity but also contains functional groups that are able to connect to the desired bio-element, the hybrid polymers appear very promising. Preparation of conducting platforms with tailored functionality such as poly(2,5-di(thienyl)pyrrole)s and poly(dithieno(3,2-b:2′,3′-d)pyrroles)s represents an excellent opportunity for achieving stable immobilization and maintaining adequate orientation of biomolecules, whilst improving the electron transfer, resulting in highly sensitive and stable biosensors. The current review briefly addresses the synthesis of hybrid thiophene-pyrrole molecules detailing several approaches and, subsequently, focuses on their application as polymeric bioimmobilization platforms for electrochemical detection of relevant bio-analytes, bio-receptors or DNA hybridization events.