Antifogging coatings for infrastructures and transparent objects have attracted much attention lately from the perspective of safety and visibility. We have developed a one-pot process to fabricate transparent composite films showing long-lasting antifogging and fast repeatable self-healing properties based on an integral blend (IB) method. This method does not require any specific pretreatments of inorganic fillers/particles. Thus, the precursor solutions could be prepared in a single step by simply mixing raw materials, e.g., poly(vinylpyrrolidone) (PVP) having different molecular weights (MWs: 55, 360, and 1300 k), nano-clay particles (NCPs), and aminoterminated organosilane (AOS). In this study, to control the degree of cross-linking between the PVP matrices and NCPs, addition of AOS as a cross-linker to the PVP matrices (weight percentage of AOS to the PVP matrices, α = 0.01−300%) was carefully controlled. Transparency and self-healing abilities/kinetics of the resulting samples were found to be strongly influenced by both the MWs of PVP and α values. Samples spin-coated with the lowest M W of PVP (55 k) and α values of 0.01−1% gave highly transparent and durable antifogging performance. For example, no fogging was observed for 7 days under >80% relative humidity, and scratches about 30 μm in width could be completely self-healed within a few hours. However, samples with α > 10% gave opaque/grayish films that did not show any self-healing abilities because of an increase in cross-linking of the matrices. The optimized precursor solution was also deposited directly onto the glass slides covered with a transparent porous silica nano-framework (SNF) by a spray-coating method. Due to the formation of the hard and superhydrophilic/hygroscopic SNF with a large surface area, durability of antifogging and self-healing properties of the composite films were moderately improved, compared to those on the flat glass slides.