The focus of this case study is the meticulous observation of urban soil pollution by heavy metals (HMs), or, alternatively, potentially toxic elements (PTEs). The study took place in the urban center of Volos, Greece. Moreover, 248 soil samples were collected during 2018–2021 (62 samples annually), while 3.65 km2 was, approximately, the study area. The breakdown of total concentrations took place for the interpretation of different soil parameters, also according to mean values and medians of the total concentrations of HMs, the following decreasing order was monitored: Mn > Zn > Cr > Ni > Cu > Pb > Co > Cd. During the 4-year study, an increasing trend of metal concentration was observed (for each year compared to the previous one). Furthermore, the imaginary triangle, which was observed, is bordered by the historic train station, the two city bus and intercity coach stations and the commercial harbor. Statistical analysis was implemented in order to interpret the exceedances of HMs concerning the Directive 86/278/EEC. Principal component analysis (PCA) is an additional technique that was conducted because of the correlations and interdependences between the HMs. A strong correlation was observed between the HMs, but mainly between Cd and Zn, which is probably due to their common origin. During the COVID-19 pandemic, significant changes in metal concentrations were observed in different parts of the city, due to the limited movement of motorized wheeled vehicles, but also due to the long operating hours of the heating systems in the residential area. Further research is needed in the future in order to identify the sources of pollution and to find possible ways to reduce it. All in all, urban soil pollution by HMs is a great conundrum of the environmental aspect of sustainability.