The fabrication of various micro-patterns on polymer insulating substrates is a current requirement in micro-electromechanical system (MEMS) and packaging sectors. In this paper, we use electrohydrodynamic jet (E-Jet) printing to create multifaceted and stable micro-patterns on a polyethylene terephthalate (PET) substrate. Initially, simulation was performed to investigate optimized printing settings in phase field physics for the usage of two distinct functional inks. A series of simulation experiments was conducted, and it was determined that the following parameters are optimised: applied pressure of 40 kPa, high pulse voltage of 1.95 kV, low dc voltage of 1.60 kV, duty cycle of 80%, pulse frequency of 60 Hz, printing height of 0.25 mm, and printing speed of 1 mm/s. Then, experiments showed that adjusting a pressure value of 40 kPa and regulating the SEMICOSIL988/1 K ink to print micro-drops on a polymer substrate with a thickness of 1 mm prevents coffee staining. The smallest measured droplet size was 200 μm. Furthermore, underfill (UF 3808) ink was driven with applied pressure to 50 kPa while other parameters were left constant, and the minimum size of linear patterns was printed to 105 μm on 0.5-mm-thick PET substrate. During the micro-drip and cone-jet regimes, the consistency and diameter of printed micro-structures were accurately regulated at a pulse frequency of 60 Hz and a duty cycle of 80%.