The church is dedicated to Saint Dimitrios and took the name "Loubardiaris" because in 1658 the following peculiar event took place. On the eve of October 26th, a thunderbolt hit the Turkish garrison commander, Yusuf Aga, who had placed a "loubarda" (def. "big canon") at the Propylaia of Acropolis because he was intending to fire upon Christian believers that Saint Dimitrios day.  The Turks, ensconced on the Acropolis, prepared to fire a cannon on the worshippers gathered in the church, but the gunner was killed by the lightning, saving the congregation. Hence its name, Loumbardiaris ('of the cannon') - considered a modern day miracle.

This 16th Century church may not be the oldest in Athens, but it is certainly one of the loveliest, with a heavy timber roof, marble floors, and emitting a permanent scent of incense. A great 1732 fresco of St. Dimitrios, astride his horse in a pose mimicked from ancient images of Alexander the Great, decorates the interior. The churchyard, with its wooden gate and bells, conjures Japan – a touch by well known modernist architect Dimitris Pikionis (1887-1968).

The designer also implemented his specific style to the renovation of the rear exterior wall, a charming piece of stonework. He was also contracted for the restoration works of the church which were carried out in 1955. On the exterior, he added marble and ceramic decorative themes to the monument. In addition, Pikionis removed the newer wall paintings and as a result, the older ones from the 18th Century were revealed. The built screen mentions the "kontakion" (a type of hymn) for the inauguration of churches.

Furthermore, leading to the church is a beautiful paved path. Thanks to its stunning location, a lot of young couples choose Agios Dimitrios Loumbardiaris the spot where they exchange their wedding vows.