Inspired by the desire to solve the energy-related issues in remote sensing applications, internet of things, wireless autonomous devices, and self-powered portable electronic devices, triboelectric nanogenerators (TENGs) have been highly promoted. However, for use in the specified applications, especially in wearable and biomedical devices, environmental-friendly materials are required. Herein, an eco-friendly pectin polymer is used as a positive triboelectric material to fabricate a TENG with excellent output performance. Working in conjunction with a polyimide, the polyimide and microarchitected pectin (MA@pectin) polymer film-based TENG (PP-TENG) generated open circuit voltage (VOC), short circuit current (ISC), and charge density (QSC) of ∼300 V, 14 μA, and 70 μC cm-2, respectively, exhibiting remarkable enhancement compared to the TENG based on polyimide/pristine pectin polymer (VOC, ISC, and QSC of 170 V, 7.6 μA, and 47 μC cm-2, respectively) under similar operating conditions. The output performance of the PP-TENG is particularly reliant on the pectin concentration, indicating an optimum concentration of 9 wt%. The improved performance of the PP-TENG was systematically analyzed and explained in terms of pectin concentration, dielectric constant, and surface roughness. Furthermore, the PP-TENG can power portable electronic devices and light-emitting diodes to prove the capability of the TENG in practical applications. The fabricated PP-TENG is anticipated to be a sustainable energy harvester via a low-cost and facile approach.