Plastics have become essential in various fields, offering multifunctionality and ease of use, where around 40% of global consumption is for packaging. However, their sustainability represents a significant challenge, as improper disposal has effects on the environment and human health. A specific challenge is the mechanical recycling of printed films, due to the presence of ink, which can contribute to the degradation of the polymer properties or cause odors. Deinking, a process to remove ink from plastic films, offers a sustainable alternative, allowing reuse of industrial plastic waste often destined for landfills or incineration. Traditional deinking methods rely on non-biodegradable surfactants, leading to environmental concerns. This study evaluates the use of bio-based surfactants, which align with sustainability goals due to their biodegradability, low toxicity, and compatibility with eco-friendly principles. Using low-density polyethylene (LDPE) films printed via flexography, the performance of five surfactants (BIO691, BA6, K15K, SRK8, SRK8P4) was tested under various conditions, including surfactant concentration, temperature, immersion time, and brushing. Employing a Design of Experiments (DoE) approach, 24 tests were conducted to optimize the deinking process. Results indicated that BIO691 and BA6 were the most effective surfactants due to their compatibility with LDPE film and ink materials. Higher temperatures significantly improved deinking efficiency, while immersion time and brushing had minimal impact. The study highlights the potential of bio-based surfactants as a sustainable solution for improving the recyclability of printed plastic films, contributing to enhanced circularity and reduced environmental impact in the plastics industry.