After leaving Hollywood, Rambova pursued a career in fashion design, opening a boutique in New York. She also traveled extensively throughout Europe, immersing herself in different cultures and artistic movements. These travels broadened her intellectual and spiritual horizons.

Rambova developed a deep interest in mysticism, spirituality, and esoteric studies. She explored various spiritual traditions, including Theosophy and astrology, seeking deeper meaning and understanding of the universe.

Rambova married Alvaro de Urzáiz y Silva, Duke of Villahermosa, a Spanish aristocrat. This marriage provided her with financial stability and allowed her to further pursue her intellectual and spiritual interests.

Rambova became involved in archaeological research, particularly related to ancient Egyptian and Near Eastern civilizations. She participated in excavations and published scholarly articles on her findings, demonstrating her intellectual curiosity and commitment to knowledge.

In her later years, Rambova continued to pursue her spiritual and intellectual interests, dividing her time between Europe and the United States. She suffered from health problems in her final years.

Natacha Rambova dies in Pasadena, California. Her legacy as a pioneering designer, an independent woman, and a seeker of knowledge continues to inspire artists and scholars.