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One-pot reactions between CuI and methyl or methyl 2-amino-isonicotinate give rise to the formation of two coordination polymers (CPs) based on double zig-zag Cu2I2 chains. The presence of a NH2 group in the isonicotinate ligand produces different supramolecular interactions affecting the Cu-Cu distances and symmetry of the Cu2I2 chains. These structural variations significantly modulate their physical properties. Thus, both CPs are semiconductors and also show reversible thermo/mechanoluminescence. X-ray diffraction studies carried out under different temperature and pressure conditions in combination with theoretical calculations have been used to rationalize the multi-stimuli-responsive properties. Importantly, a bottom-up procedure based on fast precipitation leads to nanofibers of both CPs. The dimensions of these nanofibres enable the preparation of thermo/mechanochromic film composites with polyvinylidene difluoride. These films are tens of nanometers in thickness while being centimeters in length, representing smaller thicknesses so far reported for thin-film composites. This nanomaterial integration of CPs could represent a source of alternative nanomaterials for opto-electronic device fabrication., The authors thank financial support from the Spanish Ministerio de Economía y Competitividad (MAT2016-77608-C3-1-P, MAT2016-75883-C2-2-P, MAT2010-20843-C02-01, MAT2016- 75586-C4-4-P, CTQ2016-75816-C2-1P). J. I. M. acknowledges the financial support by the “Ramón y Cajal” Program of MINECO (Grant RYC-2015-17730) and the EU via the ERCSynergy Program (Grant ERC-2013-SYG-610256 NANOCOSMOS). J. C. E. acknowledges the financial support by the “FPI-MINECO” Program of MINECO (Grant BES-2015-071534).