Radon is an increasingly common concern, mainly when it is found indoors exposing the users of the space to radiation. As a gas, radon is an element produced due to uranium decay; it emanates naturally from soil and is considered by the World Health Organization as the second most common cause of lung cancer. Several methodologies are available for mitigating the indoor radon concentration, with distinct improvements and efficiencies that need to be proved with on-site testing. The case study here presented analyzes the effect of applying a barrier membrane, covering the pavement of a ground floor room located in a historic building with a high occupancy rate, on an abnormal radon concentration evidenced by experimental data. After the barrier membrane installation, a new long-term monitoring campaign (3 months) was carried out to assess indoor radon concentration. The obtained results showed that the barrier membrane lowered the indoor radon concentration by 90%. However, the radon exposure level remained higher than the recommended level to enable safe occupation and the regular use of space. Nevertheless, as the reduction in the radon concentration was very significant by the adoption of a barrier membrane, the combination of this technical solution with other mitigation methodologies, namely including the adoption of mechanical ventilation procedures, can become a very efficient solution for radon remediation, reducing the number of air changes per hour (ACH) from 30–60 to 4–6.