In this study, we demonstrated the fabrication of multicontact hierarchical probes for the in vitro detection of serotonin levels. The basic three-dimensional (3D) bendable prototypes with 3 (C1), 6 (C2), or 9 (C3) contact surfaces were printed from polymeric resin via the digital light processing (DLP) technique. We chose ultrasonicated carbon fiber strands to transform these designs into multicontact carbon fiber electrodes (MCCFEs). The exposed carbon fiber (CF) surfaces were modified with aminopropyl alkoxysilane (APTMS), followed by the subsequent loading of palladium nanoclusters (PdNPs) to build active recording sites. CF functionalization with PdNPs was achieved by the wet chemical reduction of Pd(II) to Pd(0). The MCCFE configurations demonstrated an enhancement in the electroactive surface area and an improved voltammetric response toward 5-HT oxidation by increasing the points of the contacts (i.e., from C1 to C3). These MCCFEs are comparable to 3D-protruding electrodes as they can enable multipoint analyte detection. Along with the electrode patterns, morphological irregularities associated with both Pd-doped and undoped CFs supported the creation of proximal diffusion layers for facile mass transfer. Low detection limits of 0.8-10 nM over a wide concentration range, from 0.005 nM to 1 mM, were demonstrated. The MCCFE sensors had a relatively low standard deviation value of ∼2%. This type of sensitive and cost-effective electrochemical sensor may prove useful for collecting electrical impulses and long-term monitoring of 5-HT in vivo in addition to in vitro testing.