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Abstract The study reports novel photonic properties of Ti₃C₂T_xMXene flakes horizontally self‐assembled within cellulose nanofiber (CNF) matrix exhibiting unique bright multispectral colors combined with overall high transparency in the transmission regime. The intense reflection colors are reflected by individual flakes acting as effective micromirrors with shifts based on their subsurface positioning within the dielectric layers. Unique color appearances are controlled by an interplay of multiple bandgaps formed by constructive and destructive interferences at flake‐matrix interfaces. These colors manifest at the microscale under bright field optical microscopy, while the total physical film retains high transparency up to 85% and a typical greenish hue characteristic of the MXene content below 1% volume fraction. The diverse spectral appearance of 4 µm ultra‐thin films is ultimately controlled by the positioning of the horizontal flakes within the nanofiber matrix at diverse distances from the top surface. This work expands the understanding of thin films with assembled 2D materials within polymer matrix and their fundamental interactions creating new structural coloration functionalities with the potential for multispectral photonic applications such as camouflaging, photothermal treatment, and optical communication for flexible thin bio‐derived films. 

Abstract Polyvinylidene fluoride (PVDF) is a semicrystalline polymer used in thin‐film dielectric capacitors because of its inherently high dielectric constant and low loss tangent. Its dielectric constant can be increased by the formation and alignment of its β‐phase crystalline structure, which can be facilitated by 2D nanofillers. 2D carbides and nitrides, MXenes, are promising candidates due to their notable dielectric permittivity and ability to increase interfacial polarization. Still, their mixing is challenging due to weak interfacial interactions and poor dispersibility of MXenes in PVDF. This work explores a novel method for delaminating Ti₃C₂T_xMXene directly into organic solvents while maintaining flake size and quality, as well as the use of a non‐solvent‐induced phase separation method for producing both dense and porous PVDF‐MXene composite films. A deeper understanding of dielectric behavior in these composites is reached by examining MXenes with both mixed and pure chlorine terminations in PVDF matrices. Thin‐film capacitors fabricated from these composites display ultrahigh discharge energy density, exceeding 45 J cm⁻³with 95% efficiency. The PVDF‐MXene composites are also processed using a green and sustainable solvent, propylene carbonate.