It's now five points from five games for Pompey - not a disaster but not great when you consider three of those came in the opening game at home to Rochdale.
Jon Taylor scored what proved the only goal of the game, finishing clinically when played in on goal in the box in an attack down the Rotherham.
A new-look Pompey team that lined up with three at the back in the first half but reverted to 4-4-2 in the second period created chances but were not at their best as the Millers defended resolutely to earn their first away win in more than a season.
There were one or two surprises in the starting line-up as Kenny Jackett brought in Stuart O’Keefe and Oliver Hawkins for their debuts and welcomed Matt Clarke and Conor Chaplin back into the starting line-up.
Two other new signings, Damien McCrory and Matt Kennedy, were on the bench.
Brett Pitman and Brandon Haunstrup both had sight of goal for shots - Pitman's was just over and Haunstrup's was deflected wide for a corner.
Rotherham probably had more of the ball in the first half but found Pompey's defence hard to get past - until, that is, nine minutes before the break when Taylor ran on to a pass and fired fiercely past Luke McGee.
Jamal Lowe had an ideal chance of a quick equaliser but headed over.
There were two more debutants at the start of the second half as Nathan Thompson and Kennedy came on in place of Jack Whatmough and Chaplin, victims of Jackett's decision to try a new formation for the second half.
Lowe fired wide when a cross reached him at the far post - then a high boot that left Hawkins needing a head bandage went unpunished when Pompey felt it warranted a penalty.
Pompey perked up in the latter stages but for all their pressure could not test keeper Richard O'Donnell - and the majority of the crowd went home wet and downbeat a first home defeat of the season.
Pompey: McGee; Burgess, Whatmough (Thompson 46), Clarke; Lowe, May, O’Keefe, Haunstrup; Pitman; Chaplin (Kennedy 46), Hawkins (Naismith 70). Subs not used: Bass, McCrory, Close, Donohue
Referee: Gavin Ward
Attendance: 17,118 (436 away fans)
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