The mansion and gallery were also just south and west of the landmark Washington Monument in the Mount Vernon-Belvedere neighborhood, just north of the downtown business district and northeast of Cathedral Hill.

Upon his 1931 death, Henry Walters bequeathed the entire collection of then more than 22,000 works, the original Charles Street Gallery building, and his adjacent townhouse/mansion just across the alley to the north on West Mount Vernon Place to the City of Baltimore, "for the benefit of the public".

Highlights include two monumental 3,000-pound statues of the Egyptian lion-headed fire goddess Sekhmet on long-term loan from the British Museum; the Walters Mummy; alabaster reliefs from the palace of Ashurnasirpal II; Greek gold jewelry, including the Greek bracelets from Olbia on the shores of the Black Sea; the Praxitelean Satyr; a large assemblage of Roman portrait heads; a Roman bronze banquet couch, and marble sarcophagi from the tombs of the prominent Licinian and Calpurnian families.

In 1911, Henry Walters purchased almost 100 gold artifacts from the Chiriqui region of western Panama in Central America, creating a core collection of ancient American native art.

Among the highlights are a 7th-century carved and hammered silver bowl from Iran, (ancient Persia); a 13th-century candlestick made of copper, silver, and gold from the Mamluk era in Egypt; 16th-century mausoleum doors decorated with intricate wood carvings in a radiating star pattern; a 17th-century silk sash from the Mughal Empire in India; and a 17th-century Turkish tile with an image of the Masjid al-Haram ("Great Mosque of Mecca"), the center of Islam in Mecca, (modern Saudi Arabia).

These include a 15th-century Koran from northern India, written at the height of the Timurid Empire; a 16th-century copy of the "Khamsa of Nizami by Amir Khusraw, illustrated by a number of famous artists for the Emperor Akbar; and a Turkish calligraphy album by Sheikh Hamadullah Al-Amasi, one of the greatest calligraphers of all time.

Walters Art Museum, MS W.613 contains five Mughal miniatures from an important "Khamsa of Nizami" made for the Emperor Akbar; the rest are in London, Great Britain.

Considered one of the best collections of medieval art in the United States, the museum's holdings include examples of metalwork, sculpture, stained glass, textiles, icons, and other paintings.

Sculpted heads from the royal Abbey of St. Denis are rare surviving examples of portal sculptures that are directly connected with the origins of Gothic art in 12th-century France (accession nos.

The collection of European Renaissance and Baroque art features holdings of paintings, sculpture, furniture, ceramics, metal work, arms and armor.

The highlights include Hugo van der Goes' Donor with Saint John the Baptist, Heemskerck's Panorama with the Abduction of Helen Amidst the Wonders of the Ancient World, El Greco's Saint Francis Receiving the Stigmata, Giambattista Pittoni's Sacrifice of Polyxena, the Madonna of the Candelabra, from the studio of Raphael, Veronese's Portrait Of Countess Livia da Porto Thiene and her Daughter Porzia, El Greco's Saint Francis Receiving the Stigmata, Bernini's "bozzetto" of Risen Christ, Tiepolo's Scipio Africanus Freeing Massiva, and The Ideal City attributed to Fra Carnevale.

Highlights of the collection include Odalisque with Slave by Ingres (a second version); Claude Monet's Springtime; Alfred Sisley's panoramic view of the Seine Valley; and Édouard Manet's realist masterpiece, The Café Concert.

The museum's collection of Sèvres porcelain includes a number of pieces that were made for members of the Royal Bourbon Court at Versailles Palace outside of Paris.

Its exterior was inspired by the Renaissance-revival-style Hôtel Pourtalès in Paris and its interior was modeled after the 17th-century "Collegio dei Gesuiti" (now the Palazzo dell'Università) built by the Balbi family for the Jesuits in Genoa.

It was substantially altered in 1998–2001 by another firm of Kallmann McKinnell and Wood, Architects, to provide a four-story glass atrium, with a suspended staircase at the juncture between the older and newer buildings with a new entrance lobby along Centre Street.

[7] Throughout 2021, director Julia Marciari-Alexander, advised by union-busting law firm Shaw Rosenthal LLP,[8] refused to meet with Walters employees, stalling the advance of a wall-to-wall unionization effort.