Among various non-contact direct ink writing techniques, aerosol jet printing (AJP) stands out due to its distinct advantages, including a more adaptable working distance (2–5 mm) and higher resolution (~ 10 μm). These characteristics make AJP a promising technology for the precise customization of intricate electrical functional devices. However, complex interactions among the machine, process, and materials result in low controllability over the electrical performance of printed lines. This significantly affects the functionality of printed components, thereby limiting the broad applications of AJP. Therefore, a systematic machine learning approach that integrates experimental design, geometrical features extraction, and non-parametric modeling is proposed to achieve printing quality optimization and electrical resistivity prediction for the printed lines in AJP. Specifically, three classical convolutional neural networks (CNNs) architectures are compared for extracting representative features of printed lines, and an optimal operating window is identified to effectively discriminate better line morphology from inferior printed line patterns within the design space. Subsequently, three representative non-parametric machine learning techniques are employed for resistivity modeling. Following that, the modeling performances of the adopted machine learning methods were systematically compared based on four conventional evaluation metrics. Together, these aspects contribute to optimizing the printed line morphology, while simultaneously identifying the optimal resistivity model for accurate predictions in AJP.