The original chapel, initially dedicated to Notre-Dame, was built by Geoffroy IV, Baron of Châteaubriant, on the site where the cattle market was held from May to October until 1763. A text attests to its existence in 1263. [Threatening to fall into ruin, it was demolished in 1518, leaving only the choir of the old chapel standing. The place of worship was immediately rebuilt in a more spacious form using Châteaubriant schist (Nozay stone), based on the plans of Jean Delorme, brother of Philibert Delorme, thanks to the demolition of a neighboring house and the financial support of Jean de Laval. However, the latter's poor financial situation meant that by 1530, only the nave of the building had been built. At the death of Françoise de Foix in 1537 and Jean de Laval in 1543, the Notre-Dame chapel still lacked a framework.
It was not until 1551 that the final work was undertaken by Baron Anne de Montmorency. The dedication of the new place of worship took place ten years later, on November 5, 1561, in the presence of the coadjutor of the Bishop of Nantes, and the name of Notre-Dame was changed to Saint-Nicolas, for an unknown reason. On the same day, the body of Jean de Laval, then encased in a lead reliquary, was transported from the castle chapel to the new building. Jean de Laval had wished to see the chapel erected as a collegiate church, but this wish was not granted. However, the building, as vast as a church, shared the honors of worship with the Church of Saint-Jean de Béré, which was then the parish church of the town, until the Revolution. Indeed, the Saint-Nicolas chapel, although of undeniable architectural value, was not suitable for worship in a parish as large as that of Châteaubriant. Nevertheless, in the 15th and 16th centuries, masses, vespers, and many ceremonies were held in the chapel for reasons of convenience, as it was closer to the town of Châteaubriant, while baptisms were all celebrated at Saint-Jean de Béré.
At the end of the 19th century, the church, which became the parish seat in 1801, was completely rebuilt.
The architect Eugène Boismen drew up the plans, inspired by those of the Saint-Nicolas basilica in Nantes, one of the first neo-Gothic projects in France, which was beginning to inspire architects throughout the west of the country.
The foundation stone was blessed on April 25, 1875, by Bishop Fournier of Nantes. The choir, sacristies, transept, and five bays were only completed at the time of the consecration, which was performed by his successor, Bishop Le Coq, on February 1, 1881. The foundations of the bell tower and the remaining bay began in June 1892, based on plans by architect François Bougoüin. The tower and spire were completed in August 1894.