Healable films with structural color are highly desirable and have a variety of potential applications. However, combining structural color with self-healing properties to obtain new functional materials is a big challenge in current research. Herein, we present the first example of a color tunable, ultrathin film that can self-heal in response to external mechanical abrasion. It is designed based on intermolecular hydrogen bonding interaction; the synthetic strategy involves spin-coating of poly(acrylic acid) (PAA) and chitosan (CS). The successful preparation of ultrathin, healable, structural color films provides a new type of biomimetic material.One of the characteristic features of living systems is structural color, which can be detected in the outer shells of jewel beetles, wings of butterflies and on many other insects.[1] The structural color originates from spectrally selective reflection of visible light from a periodic modulation of refractive index rather than pigment, dye or luminescence. Inspired by natural biological structures, photonic crystals (PhCs), which are composite structures with a periodic arrangement of refractive index in one dimension, [2] two dimensions, [3] and three dimensions, [4] have been designed and fabricated. Recently, they have been gradually applied in a myriad of applications such as optical devices, [5] sensing materials, [6] display technologies, [7] solar cells [8] and so on. [9] One-dimensional photonic crystals (1DPhCs) have the simplest structures and are easy to handle because of their simple structures composed of alternately stacked thin-film layers with high and low refractive indices. [10] The dynamic coloration is generally achieved either by changing the thickness of the multilayers or the refractive index of individual layers through chemical reactions. [11] Although PhCs have substantial potential applications in the development of advanced functional materials, accidental scratches on optical films change the way light is transmitted and can even cause severe light scattering. Such scratches on optical films have to be healed to restore their original optical functions for further applications.[12] Ideally, if we can mimic the living biological systems more closely and endow the materials with self-healing properties, the designed materials will have extended service lives, which can facilitate their maintenance and increase their reliability with stable functionality. [13] However, combining structural color with self-healing property is an enormous challenge, and there is no report on this field to date.In general, polymers have great potential for self-healing due to the high mobility of the polymer chains under physiological conditions. Polyelectrolyte multilayers have a pronounced self-healing effect due to their mobility in response to environmental change. External stimuli such as pH, ionic strength, temperature, light, etc. affect ionization of the functional groups of the polyelectrolytes, which makes the polyelectrolyte multilayers st...