The main units are:
- The very rare – among the earliest artifacts in the Collection – Medieval Venetian helmets of the fourteenth and fifteenth centuries, which were discovered in 1840 in a vaulted casemate in the wall of the fortress of Chalkis.
- A large number of weapons belonging to eponymous freedom fighters of the 1821 War of Independence, either inherited from their descendants or booty or supplied by the Philhellenes. Among these are weapons of the klephts and armatoloi (armed irregulars) under Zervas and Tzavelas, of those who battled at sea such as Lambros Katsonis, Konstantinos Kanaris and Andreas Miaoulis, and of the freedom fighters Theodoros Kolokotronis, Ioannis Makrygiannis, Georgios Karaiskakis, Athanasios Diakos, Nikitas Stamatelopoulos (Nikitaras). There are weapons also of the soldier in the Sacred Brigade Konstantinos Xenokratis, the member of the Philike Hetaireia Georgakis Olympios, the Phanariot Princes of the Danubian Principalities, Philhellenes such as Lord Byron, as well as of Ali Pasha of Ioannina.
- Weaponry from the Cretan Uprising and the Macedonian Struggles, the Balkan Wars, the Asia Minor Campaign and the two World Wars.
- Weapons of diverse provenance from the private collection of King George I, with pieces of superb quality of Abyssinian and Indo-Persian provenance, as well as royal hunting equipment.