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According to Deadline Hollywood, the How I Met Your Mother star and Emmy host is the first major actor to join the live-action/CGI hybrid.
Harris will likely team with Jonathan Winters, who has reportedly signed to voice Papa Smurf in the film.
Scooby-Doo director Raja Gosnell is to helm the feature, based on the tiny blue cartoon characters best known through the popular 1980s animated series.
More: Neil Patrick Harris, Movies
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