The concentration distribution of anthropocentric pollutants is favored by urban densification, affecting the micrometeorology in big cities. To examine this condition, chaos theory was applied to time series of measurements of urban meteorology and pollutants of six communes of the Metropolitan Region of Santiago de Chile, in two periods: 2010–2013 and 2017–2020. Each commune contributes, per period, six different time series: three for the meteorological variables (temperature, relative humidity, and magnitude wind speed) and three for the atmospheric pollutant concentrations (PM10, PM2.5, and CO). This qualitative study corroborates that each of the time series is chaotic through the calculation of chaotic parameters: Lyapunov exponent, correlation dimension, Hurst coefficient, correlation entropy, Lempel–Ziv complexity and fractal dimension. The variation in the chaotic parameters between the two periods can be interpreted in relation to the roughness change due to urban densification. More specific parameters, constructed from the Kolmogorov entropies and the fractal dimensions of the time series, show modifications due to the increase in the built surface in the most current period. This variation also extends to micrometeorology, as is clear from the Lempel–Ziv complexity and the Hurst coefficient. The qualitative picture constructed using chaos theory reveals that human interaction with nature affects diversity and sustainability and generates irreversible processes.