Apparently, as per Reddit, the director kept wanting her to look more scared in her initial scenes; explaining the horror of being kidnapped and imprisoned in her own home by a strange man. She kept pleading "But it's Robert Redford"!
If you like the espionage and unique feel of films of that era though, you can't do much better than Francis Ford Coppola's 'The Conversation', starring a wonderfully morose Gene Hackman. A very worthy Palme D'Or winner in '74.
Fred Zinnemann's 'The Day of the Jackal' in '73 is also a high-point for espionage-thrillers of the decade.