Krause attended and played high school football at Bendle High School in Burton, Michigan and earned all-state honors in basketball, football, baseball and track. Known for once scoring 54 points in a basketball game, he was one of the few in his high school to ever receive an athletic scholarship.
Krause also played baseball at Iowa. As a sophomore, he earned All-American honors and was drafted into the major leagues, but he turned down the offer. Krause's chances to play professional baseball were ended when he injured his shoulder in his junior year playing football against the University of Michigan.
Krause was drafted in the second round of the 1964 NFL Draft by the Washington Redskins. In his rookie season, he led the NFL in interceptions with 12, including interceptions in seven straight games, and was named to the All-NFL first team. He was named to his first of eight Pro Bowls and was second only to teammate Charley Taylor for the NFL Rookie of the Year award.
Krause played with the Vikings until he retired after the 1979 season. During that time, he was one of 11 players to play in all four of the Vikings Super Bowl appearances (Super Bowl IV, VIII, IX, and XI). Krause recorded an interception in Super Bowl IV and a fumble recovery in Super Bowl IX.
Krause was often referred to as the Vikings "Center Fielder" because of his success as an interscholastic baseball player and his ability to catch interceptions.
He currently holds the all-time interception record in the NFL with 81, which he returned for 1,185 yards and three touchdowns. He acquired the record in 1979 against the Los Angeles Rams, in the second quarter of a 27-21 overtime loss with his 81st interception coming in the final period. The previous record of 79 was held by Emlen Tunnell, another former Hawkeye who played for the New York Giants and the Green Bay Packers from 1948 to 1961.
Krause recovered 19 fumbles, returning them for 163 yards and three touchdowns. Krause only missed two games due to injuries in 16 seasons.
In 1994, Krause was elected to the Board of County Commissioners for Dakota County, Minnesota. He served for twenty years he did not seek re election in 2014. 
Currently, Krause is involved in real estate development and insurance, and he owns several restaurants, including the Dairy Delite in Lakeville, Minnesota. He previously owned a golf course in Elk River, Minnesota.
Krause is married to his wife, Pam, and has three children: two daughters (Mandi and Zendi) and one son (Blair).
In 1996, Pam Krause was severely injured in a car accident near their home in Lakeville, Minnesota when she was hit by a truck. She spent five and a half months in a coma, but survived and is recuperating.