Looks like the variable OverallTime is a string. you cannot compare a string and an int;
Also, timeSinceLevelLoad is a float, you should really leave it as such otherwise your time will be truncated into whole seconds.
Instead you can just omit the variable completely and use:
if(Time.timeSinceLevelLoad > PlayerPrefs.GetInt("HighScore")){
// new high score!
PlayerPrefs.SetFloat("HighScore", Time.timeSinceLevelLoad;
PlayerPrefs.Save();
}