The surface properties of biomaterials interact directly with biological systems, influencing cellular responses, tissue integration, and biocompatibility. Surface topography plays a critical role in cardiac tissue engineering by affecting electrical conductivity, cardiomyocyte alignment, and contractile function. Current methods for controlling surface properties and topography in cardiac tissue engineering scaffolds are limited, expensive, and lack precision. This study introduces a low-cost, one-step degradation process to create scaffolds with well-defined micro-grooves from multilayered 3D printed poly(lactic acid)/thermoplastic polyurethane composites. The approach provides control over erosion rate and surface morphology, allowing easy tuning of scaffold topographical cues for tissue engineering applications. The findings reported in this study provide a library of easily tuneable scaffold topographical cues. A strong dependence of neonatal rat cardiomyocyte (NRCM) contact guidance with the multilayers' dimension and shape in partially degraded polylactic acid (PLA)/thermoplastic polyurethane (TPU) samples is observed. NRCMs cultured on samples with a layer thickness of 13 ± 2 µm and depth of 4.7 ± 0.2 µm demonstrate the most regular contractions. Hence, the proposed fabrication scheme can be used to produce a new generation of biomaterials with excellent controllability determined by multilayer thickness, printing parameters, and degradation treatment duration.