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The question is complex because Princess Mononoke was released in Japan in 1997, but the English-language dub featuring international stars was released in the U.S. in 1999. In an international context, the most famous actor is typically considered to be one of the major names in the English dub, as the Japanese cast's fame is primarily regional.
The most famous actor in the film's international English-language cast at the time of the original 1997 Japanese release, and certainly by the 1999 English-dub release, was arguably Gillian Anderson, who voiced the wolf goddess, Moro.
At the time of the film's original 1997 release, and during the production of the English dub, Gillian Anderson was at the height of her fame as a global television icon, which made her more widely recognizable worldwide than her co-stars.
Gillian Anderson's fame was almost entirely driven by her starring role in a massive television hit, for which she was heavily decorated in 1997.
Television: The X-Files (1993–2002)
Notable Films (Around the Time of the Dub):
Several other major stars in the English dub were at or near the peak of their fame in the late 1990s, including:
The summary dismisses the Japanese cast as 'regional,' but Hisaya Morishige (Okkoto) was a legendary actor in Japan (Order of Culture recipient), and Akihiro Miwa (Moro) is a major cultural icon. Mentioning them would provide a more complete 'global' picture, though the focus on the English dub is appropriate for an English query.
Jada Pinkett Smith (voice of Toki) was also a major star in 1997-1999 (Scream 2, Nutty Professor, marriage to Will Smith), comparable in fame to the others listed.
For the English-speaking world, the most famous actor in Princess Mononoke at the time of its release (US dub, 1999) was Gillian Anderson (Moro), who was a global icon due to The X-Files. Billy Bob Thornton (Jigo) was also highly prominent, having recently won an Oscar for Sling Blade (1996) and starred in Armageddon (1998). Claire Danes (San) was a major teen star following Romeo + Juliet (1996). In the original Japanese cast (1997), the most famous figure was likely Hisaya Morishige (Okkoto), a legendary stage and film actor who received the Order of Culture, or Akihiro Miwa (Moro), a renowned singer and cultural icon.